Olefin derived copolymer

ABSTRACT

The present invention relates to an olefin derived copolymer and a thermoplastic resin composition using the olefin derived copolymer satisfying the following (1) and (2): (1) tensile strength at break measured based on JIS K6251 is 2.0 or less MPa; and (2) tensile elongation at break EB (%) of a resin composition obtained satisfies the following relational expression (expression 1) and (expression 2), when blended with a polypropylene derived resin that has 20 degree C. xylene soluble component of not more than 20 wt %.
 
 R [3/5]− R [2/6]≧0.15  (expression 1)
 
 S [2/6]≧−800  (expression 2)
 
     (R[3/5] and R[2/6] are obtained by the following methods: a curve is obtained by plotting tensile elongation at break EB (%) (based on JIS K6251) of resin composition taken as vertical axis, and weight part rate Pa of a content of an olefin derived copolymer contained in a resin composition taken as horizontal axis; a multiple regression curve in section regions of Pa=0.30-0.50 and Pa=0.20-0.60 (Pa represents content weight percentage of an olefin derived copolymer contained in a resin composition) of a multiple regression expression obtained by quintic multiple regression of the curve is obtained; R[3/5] and R[2/6] are defined as multiple correlation coefficients of a primary straight line obtained by approximating of the multiple regression curve by method of least squares. S[2/6] represent a gradient of a primary straight line (expression) obtained by approximating the above-mentioned multiple regression curve by a method of least squares in section region of Pa=0.20-0.60. In addition, in the above-mentioned multiple regression expression, it is indispensable that data at least seven points Pa=0.00, 0.20, 0.30, 0.40, 0.50, 0.60 and 0.70 are contained. Furthermore, when data at points of number beyond above case are contained, it is indispensable that total Pa values exist at 0.10 or less of fixed interval mutually.

This application is the National phase of International ApplicationPCT/JP00/04803, filed 17 Jul. 2000, which designated the U.S. and thatInternational Application was not published under PCT Article 21(2) inEnglish.

TECHNICAL FIELD

The present invention relates to an olefin derived copolymer and athermoplastic resin composition. Furthermore in detail, the presentinvention relates to an olefin derived copolymer that may provide athermoplastic resin composition with outstanding flexibility,transparency, resistance to whitening, scratch resistance, and tensileelongation characteristics, and excellent balance of flexibility, heatresistance, and weather resistance, and outstanding surface characterstability and relates to a thermoplastic resin composition therewith.

BACKGROUND TECHNOLOGY

Soft vinyl chloride resin is a material that has excellent performances,such as outstanding flexibility, heat resistance, scratch resistance,and transparency, and is widely used in many fields. However, in recentyears materials responsible for environmental problem comes to berequired, and a demand for substitution to non-soft vinyl chloridematerial is increasing in use where soft vinyl chloride has beenconventionally used. In such a background, as a soft material consistingonly of olefin component, a resin composition comprisingethylene-α-olefin copolymer and crystalline polypropylene resin is knownas thermoplastic resin compositions (JP,7-102126,A etc.) excellent inflexibility, transparency, mechanical strength, resistance to whitening,and cold resistance. However, a problem of stickiness of surfaceoriginated in ethylene-α-olefin copolymer remains as is described inJP,8-301927,A, and the material is not provided in practical use.

On the other hand, as a trial improving these stickiness, although amethod of cross-linking with electron beam or peroxide in copolymercomprising ethylene-α-olefin etc. is also proposed (JP,8-301927,A,JP,9-104720,A), still sufficient result is not given. On the other hand,a tacky adhesion sheet or film comprises base material films, such asvinyl chloride resin, polyethylene, and polypropylene etc. and pressuresensitive adhesive layers with acrylics derived or rubber derived maincomponents. These tacky adhesion sheets or films are often used assurface protection film and a tape for fixation and union at the time ofpackaging and packing in order to prevent crack and soils during storageor transportation of materials, such as construction materials,stainless steel, aluminum board, home electronics, precision instrument,and car, or in order to prevent getting damaged in case of secondaryprocessings, such as bend processing and press processing. However, inrecent years although a tacky adhesion film made of vinyl chloride resingroup material is excellent in performances, such as flexibility, heatresistance, scratch resistance, and transparency, a conversion demandinto non-chlorine derived material is increasing in material demands forenvironmental problem. On the other hand, although a tacky adhesion filmmade of polyethylene and polypropylene group material is alsoconventionally used in some fields as a non-chlorine derived material, asufficient result is not given, for example in the field where advancedflexibility, such as close contact to an objects to be covered andductility at the time of processing, is required. And although a trialin which ethylene-α-olefin copolymer with excellent flexibility is addedto polyethylene or polypropylene is also carried out for the purpose ofproviding flexibility in response to this situation, a problem isinduced that heat resistance is greatly spoiled or surface stickinessarises, if excessive amount of this ethylene-α-olefin copolymer is addedin order to raise flexibility. Moreover, a material, as non-chlorinederived material using olefin derived polymer, in which styrene derivedblock copolymer is blended into polypropylene is inadequate inflexibility compared with vinyl chloride resin. And since styrene blockunit is contained in large quantities, depending on used condition,weather resistance at the time of outdoor exposure and especiallyultraviolet radiation stability are not necessarily enough to give apossible problem of decrease in physical properties in use out in thefields.

SUMMARY OF THE INVENTION

In this situation, as a result of wholehearted investigation performedby the present inventors in search of a composition that has outstandingflexibility, transparency, resistance to whitening, scratch resistance,and tensile elongation characteristics, and also has an outstandingbalance of flexibility, heat resistance, and weatherproof when blendedwith polyolefin resin, and at the same time of a new modified materialthat can prevent a stickiness phenomenon, as in weathering test of carinterior, after high temperature heat resistance examination, it wasfound out that the above-mentioned subject is solved by using a newolefin derived copolymer with certain specific physical properties.Moreover, by using a base material sheet or film containing athermoplastic resin composition of the present invention, it was foundout that the above-mentioned subject is solved to complete the presentinvention.

A subject solved by the present invention is to provide an olefinderived copolymer that consists only of olefin without chlorine and thatgives a thermoplastic resin composition having outstanding flexibility,transparency, resistance to whitening, scratch resistance, and tensileelongation characteristics, and an excellent balance in flexibility,heat resistance, and weather resistance, and that does not generatedecrease in surface character after heating promoted examination, and toprovide a thermoplastic resin composition using the olefin derivedcopolymer.

Namely, the present invention relates to an olefin derived copolymer anda thermoplastic resin composition using the olefin derived copolymersatisfying the following (1) and (2):

-   -   (1) tensile strength at break measured based on JIS K6251 is 2.0        or less MPa; and    -   (2) tensile elongation at break EB (%) of a resin composition        obtained satisfies the following relational expression        (expression 1) and (expression 2), when blended with a        polypropylene derived resin that has 20 degree C. xylene        solluble component of not more than 20 wt %.        R[3/5]−R[2/6]≧0.15  (expression 1)        S[2/6]≧−800  (expression 2)    -   (R[3/5] and R[2/6] are obtained by the following methods:    -   a curve is obtained by plotting tensile elongation at break EB        (%) (based on JIS K6251) of resin composition taken as vertical        axis, and weight part rate Pa of a content of an olefin derived        copolymer contained in a resin composition taken as horizontal        axis; a multiple regression curve in section regions of        Pa=0.30-0.50 and Pa=0.20-0.60 (Pa represents content weight        percentage of an olefin derived copolymer contained in a resin        composition) of a multiple regression expression obtained by        quintic multiple regression of the curve is obtained;    -   R[3/5] and R[2/6] are defined as multiple correlation        coefficients of a primary straight line obtained by        approximating of the multiple regression curve by method of        least squares. S[2/6] represents a gradient of a primary        straight line (expression) obtained by approximating the        above-mentioned multiple regression curve by a method of least        squares insection region of Pa=0.20-0.60. In addition, in the        above-mentioned multiple regression expression, it is        indispensable that data at least seven points Pa=0.00, 0.20,        0.30, 0.40, 0.50, 0.60 and 0.70 are contained. Furthermore, when        data at points of number beyond above case are contained, it is        indispensable that total Pa values exist at 0.10 or less of        fixed interval mutually.

THE BEST MODE FOR CARRYING OUT THE INVENTION

An olefin derived copolymer of the present invention means copolymersobtained by copolymerizing two or more kinds of monomer componentschosen from ethylene, α-olefins with 3-20 carbons, polyene compounds,cyclic olefins, and vinyl aromatic compounds, and polymers or polymerswith copolymer-like structure obtained by homopolymerizing thesemonomers. As examples of monomers that constitute the olefin derivedcopolymers, monomers of following (a)-(d) are mentioned.

(a) α-Olefins

Linear and branched α-olefins are contained as α-olefins with 3-20carbons used in the present invention. For example, as linear α-olefins,propylene, 1-butene, 1-pentene, 1-hexene, 1-heptene, 1-octene, 1-nonene,1-decene, 1-undecene, 1-dodecene, 1-tridecene, 1-tetradecene,1-pentadecene, 1-hexadecene, 1-hptadecene, 1-octadecene, 1-nanodecene,1-eicocene, etc. are mentioned; as branched α-olefins,3-methyl-1-butene, 3-methyl-1-pentene, 4-methyl-1-pentene,2-ethyl-1-hexene, 2,2,4-trimethyl-1-pentene etc. are mentioned; andpreferably linear propylene, 1-butene, 1-pentene, 1-hexene, 1-octene,1-decene, etc. are mentioned.

(b) Polyene Compounds

As a polyene compounds suitably used in the present invention, so-calledconjugated polyene compounds in which one single bond is insertedbetween double bonds, and the other non-conjugated polyene compounds arecontained. As conjugated polyene compounds, aliphatic conjugated polyenecompounds and cycloaliphatic conjugated polyene compounds etc. arementioned. As aliphatic conjugated polyene compounds, linear aliphaticconjugated polyene compounds and branched aliphatic conjugated polyenecompounds are contained. Moreover, aliphatic conjugated polyenecompounds and cycloaliphatic conjugated polyene compounds may containalkoxy group, aryl group, aryloxy group, aralkyl group, and aralkyl oxygroup, etc.

As aliphatic conjugated polyene compounds, for example, 1,3-butadiene,isoprene, 2-ethyl-1,3-butadiene, 2-propyl-1,3-butadiene, 2-isopropyl-1,3-butadiene, 2-hexyl-1,3-butadiene, 2,3-dimethyl-1,3-butadiene,2,3-diethyl-1,3-butadiene, 2-methyl-1,3-pentadiene,2-methyl-1,3-hexadiene, 2-methyl-1,3-octadiene, 2-methyl-1,3-decadiene,2,3-dimethyl-1,3-pentadiene, 2,3-dimethyl-1,3-hexadiene,2,3-dimethyl-1,3-octadiene, 2,3-dimethyl-1,3-decadiene, etc. arementioned. As cycloaliphatic conjugated polyene compounds, for example,2-methyl-1,3-cyclopentadiene, 2-methyl-1,3-cyclohexadiene,2,3-dimethyl-1,3-cyclopentadiene, 2,3-dimethyl-1,3-cyclohexadiene,2-chloro-1,3-butadiene, 2,3-dichloro-1,3-butadiene,1-fluoro-1,3-butadiene, 2-chloro-1,3-pentadiene,2-chloro-1,3-cyclopentadiene, 2-chloro-1,3-cyclohexadiene, etc. arementioned.

As non-conjugated polyene compounds, aliphatic non-conjugated polyenecompounds, cycloaliphatic non-conjugated polyene compounds and aromaticnon-conjugated polyene compounds, etc. are mentioned. As aliphaticnon-conjugated polyene compounds, linear aliphatic non-conjugatedpolyene compounds and branched aliphatic non-conjugated polyenecompounds are contained. Moreover, aliphatic non-conjugated polyenecompounds, cycloaliphatic non-conjugated polyene compounds, and aromaticnon-conjugated polyene compounds may contain alkoxy group, aryl group,aryloxy group, aralkyl group, aralkyl oxy group, etc. As aliphaticnon-conjugated polyene compounds, for example 1,4-hexadiene,1,5-hexadiene, 1,6-heptadiene, 1,6-octadiene, 1,7-octadiene,1,8-nonadiene, 1,9-decadiene, 1,13-tetradecadiene, 1,5,9-decatriene,3-methyl-1,4-hexadiene, 4-methyl-1,4-hexadiene, 5-methyl-1,4-hexadiene,4-ethyl-1,4-hexadiene, 3-methyl-1,5-hexadiene.3,3-dimethyl-1,4-hexadiene, 3,4-dimethyl-1,5-hexadiene,5-methyl-1,4-heptadiene, 5-ethyl-1,4-heptadiene,5-methyl-1,5-heptadiene, 6-methyl-1,5-heptadiene,5-methyl-1,5-heptadiene, 3-methyl-1,6-heptadiene,4-methyl-1,6-heptadiene, 4,4-dimethyl-1,6-heptadiene,4-ethyl-1,6-heptadiene, 4-methyl-1,-octadiene, 5-methyl-1,4-octadiene,4-ethyl-1,4-octadiene, 5-ethyl-1,4-octadiene, 5-methyl-1,5-octadiene,6-methyl-1,5-octadiene, 5-ethyl-1,5-octadiene, 6-ethyl-1,5-octadiene,6-methyl-1,6-octadiene, 7-methyl-1,6-octadiene, 6-ethyl-1,6-octadiene,6-propyl-1,6-octadiene, 6-butyl-1,6-octadiene, 4-methyl-1,4-nonadiene,5-methyl-1,4-nonadiene, 4-ethyl-1,4-nonadiene, 5-ethyl-1,4-nonadiene,5-methyl-1,5-nonadiene, 6-methyl-1,5-nonadiene, 5-ethyl-1,5-nonadiene,6-ethyl-1,5-nonadiene, 6-methyl-1,6-nonadiene, 7-methyl-1,6-nonadiene,6-ethyl-1,6-nonadiene, 7-ethyl-1,6-nonadiene, 7-methyl-1,7-nonadiene,8-methyl-1,7-nonadiene, 7-ethyl-1,7-nonadiene, 5-methyl-1,4-decadiene,5-ethyl-1,4-decadiene, 5-methyl-1,5-decadiene, 6-methyl-1,5-decadiene,5-ethyl-1,5-decadiene, 6-ethyl-1,5-decadiene, 6-methyl-1,6-decadiene,6-ethyl-1,6-decadiene, 7-methyl-1,6-decadiene, 7-ethyl-1,6-decadiene,7-methyl-1,7-decadiene, 8-methyl-1,7-decadiene, 7-ethyl-1,7-decadiene,8-ethyl-1,7-decadiene, 8-methyl-1,8-decadiene, 9-methyl-1,8-decadiene,8-ethyl-1,8-decadiene, 6-methyl-1,6-undecadiene,9-methyl-1,8-undecadiene, 6,10-dimethyl-1,5,9-undecatriene,5,9-dimethyl-1,4,8-decatriene, 4-ethylidene-8-methyl-1,7-nonadiene,13-ethyl-9-methyl-1,9,12-pentadecatriene,5,9,13-trimethyl-1,4,8,12-tetradecadiene,8,14,16-trimethyl-1,7,14-hexadecatriene,4-ethylidene-12-methyl-1,11-pentadecadiene, etc. may be mentioned. Ascycloaliphatic non-conjugated polyene compounds, for example, vinylcyclohexene, 5-vinyl-2-norbornene, 5-ethylidene-2-norbornene,5-methylene-2-norbornene, 5-isopropenyl-2-norbornene, cyclo hexadiene,dicyclo pentadiene, cyclo octadiene, 2,5-norbornenadiene,2-methyl-2,5-norbornenadiene, 2-ethyl-2,5-norbornenadiene,2,3-diisopropylidene-5-norbornene, 2-ethylidene-3-isopropylidene-5-norbornene, 6-chloro methyl-5-isopropenyl-2-norbornene,1,4-divinyl cyclohexane, 1,3-divinyl cyclohexane, 1,3-divinylcyclopentane, 1,5-divinyl cyclooctane, 1-allyl-4-vinyl cyclohexane,1,4-diallyl cyclohexane, 1-allyl-5-vinylcyclooctane,1,5-diallylcyclooctane, 1-allyl-4-isopropenylcyclohexane,1-isopropenyl-4-vinylcyclohexane, 1-isopropenyl-3-vinyl cyclopentane,methyl tetra hydro indene, etc. may be mentioned. As aromaticnon-conjugated polyene compounds, for example, divinylbenzene, vinylisopropenyl benzene, etc. may be mentioned.

(C) Cyclic Olefin Compounds

As cyclic olefins that may be used for constituting olefin polymers inthe present invention, for example, norbornene, 5-methyl norbornene,5-ethyl norbornene, 5-propyl norbornene, 5,6-dimethyl norbornene,1-methyl norbornene, 7-methyl norbornene, 5,5,6-trimethyl norbornene,5-phenyl norbornene, 5-benzyl norbornene, 5-ethylidene norbornene,5-vinyl norbornene, 1,4,5,8-dimethano-1,2,3,4,4a,5,8,8a-octahydronaphthalene, 2-methyl-1,4,5,8-dimethano-1,2,3,4,4a,5,8,8a-octahydronaphthalene, 2-ethyl-1,4,5,8-dimethano-1,2,3,4,4a,5,8,8a-octahydronaphthalene, 2,3-dimethyl-1,4,5,8-dimethano-1,2,3,4,4a,5,8,8a-octahydronaphthalene, 2-hexyl 1,4,5,8-dimethano-1,2,3,4,4a,5,8,8a-octahydronaphthalene, 2-ethylidene-1,4,5,8-dimethano-1,2,3,4,4a,5,8,8a-octahydronaphthalene, 2-fluoro-1,4,5,8-dimethano-1,2,3,4,4a,5,8,8a-octahydronaphthalene, 1,5-dimethyl-1,4,5,8-dimethano-1,2,3,4,4a,5,8,8a-octahydronaphthalene, 2-cyclohexyl-1,4,5,8-dimethano-1,2,3,4,4a,5,8,8a-octahydronaphthalene, 2,3-dichloro-1,4,5,8-dimethano-1,2,3,4,4a,5,8,8a-octahydronaphthalene, 2-isobutyl-1,4,5,8-dimethano-1,2,3,4,4a,5,8,8a-octahydronaphthalene, 1,2-dihydro dicyclopentadiene, 5-chloro norbornene,5,5-dichloro norbornene, 5-fluoro norbornene,5,5,6-trifluoro-6-trifluoromethylnorbornene, 5-chloromethyl norbornene,5-methoxy norbornene, 5,6-dicarboxyl norbornene anhydrate, 5-dimethylamino norbornene, 5-cyano norbornene, cyclopentene, 3-methylcyclopentene, 4-methyl cyclopentene, 3,4-dimethylcyclopentene,3,5-dimethylcyclopentene, 3-chloro cyclopentene, cyclohexene, 3-methylcyclohexene, 4-methyl cyclohexene, 3,4-dimethyl cyclohexene, 3-chlorocyclohexene, cycloheptene, etc. may be mentioned.

(d) Vinyl Aromatic Compounds

As a vinyl aromatic compounds which can be used for constituting olefinpolymer in the present invention, for example, styrene, α-methylstyrene, p-methyl styrene, vinyl xylene, monochloro styrene, dichlorostyrene, monobromo styrene, dibromo styrene, fluoro styrene,p-tert-butyl styrene, ethyl styrene, vinyl naphthalene, etc. may bementioned.

Furthermore, in the present invention in the light of achievement ofsurface character stability and flexibility, and achievement of abalance of flexibility, heat resistance, and weather resistance ofthermoplastic resin composition that is one of the objects of thepresent invention, polymers that comprise combination of specificmonomers chosen from the above-mentioned monomers are preferable, andcombination of following (1)-(19) may be mentioned as examples ofpreferable polymers;

-   -   (1) olefin derived copolymers in which ethylene and α-olefin        with 3-20 carbons are indispensable, and with them one or more        kinds of monomer components chosen from polyene compounds,        cyclic olefins, and vinyl aromatic compounds are arbitrarily        copolymerized,    -   (2) olefin derived copolymers in which ethylene and α-olefin        with 4-20 carbons are indispensable, and with them one or more        kinds of monomer components chosen from polyene compounds,        cyclic olefins, and vinyl aromatic compounds are arbitrarily        copolymerized,    -   (3) olefin derived copolymers in which ethylene, propylene, and        α-olefins with 4-20 carbons are indispensable components, and        with them one or more kinds of monomer components chosen from        polyene compounds, cyclic olefins, and vinyl aromatic compounds        are arbitrarily copolymerized,    -   (4) olefin derived copolymers in which propylene and α-olefins        with 4-20 carbons are indispensable components, and one or more        kinds of monomer components chosen from polyene compounds,        cyclic olefins, and vinyl aromatic compounds are arbitrarily        copolymerized,    -   (5) olefin derived copolymers that consist of ethylene and        α-olefins with 4-20 carbons,    -   (6) olefin derived copolymers that consist of ethylene α-olefins        with 4-20 carbons and polyene compounds,    -   (7) olefin derived copolymers that consist of ethylene,        α-olefins with 4-20 carbons, and cyclic olefin compounds,    -   (8) olefin derived copolymers that consist of ethylene,        α-olefins with 4-20 carbons, and vinyl aromatic compounds,    -   (9) olefin derived copolymers that consist of ethylene,        α-olefins with 4-20 carbons, polyene compounds, and vinyl        aromatic compounds,    -   (10) olefin derived copolymers that consist of ethylene,        propylene, and α-olefins with 4-20 carbons,    -   (11) olefin derived copolymers that consist of ethylene,        propylene, α-olefins with 4-20 carbons, and polyene compounds,    -   (12) olefin derived copolymers that consist of ethylene,        propylene, α-olefins with 4-20 carbons, and cyclic olefin        compounds,    -   (13) olefin derived copolymers that consist of ethylene,        propylene, α-olefins with 4-20 carbons, and vinyl aromatic        compounds,    -   (14) olefin derived copolymers that consist of ethylene,        propylene, α-olefins with 4-20 carbons, polyene compounds, and        vinyl aromatic compounds,    -   (15) olefin derived copolymers obtained by copolymerizing        propylene and α-olefins with 4-20 carbons,    -   (16) olefin derived copolymers that consist of propylene,        α-olefins with 4-20 carbons, and polyene compounds,    -   (17) olefin derived copolymers that consist of propylene,        α-olefins with 4-20 carbons, and cyclic olefin compounds,    -   (18) olefin derived copolymers that consist of propylene,        α-olefins with 4-20 carbons, and vinyl aromatic compounds, and    -   (19) olefin derived copolymers that consist of propylene,        α-olefins with 4-20 carbons, polyene compounds, and vinyl        aromatic compounds.

Among the above-mentioned combinations, following combinations arepreferable in the light of low temperature resistance of olefin derivedcopolymers obtained and thermoplastic resin compositions constituted byincluding them.

-   -   (2) olefin derived copolymers in which ethylene and α-olefins        with 4-20 carbons are indispensable, and with them one or more        kinds of monomer components chosen from polyene compounds,        cyclic olefins, and vinyl aromatic compounds are arbitrarily        copolymerized,    -   (3) olefin derived copolymers in which ethylene, propylene, and        α-olefins with 4-20 carbons are indispensable components, and        with them one or more kinds of monomer components chosen from        polyene compounds, cyclic olefins, and vinyl aromatic compounds        are arbitrarily copolymerized.

Among the above-mentioned combinations, following combinations arepreferable in the light of a balance of flexibility, heat resistance,and weather resistance of thermoplastic resin compositions obtained andof a molded body containing the thermoplastic resin compositionsobtained.

-   -   (9) olefin derived copolymers that consist of ethylene,        α-olefins with 4-20 carbons,    -   (10) olefin derived copolymers that consist of ethylene,        propylene, and α-olefins with 4-20 carbons.

Olefin derived copolymers of the present invention are olefin derivedcopolymers characterized by satisfying requirements of following (1) and(2):

-   -   (1) Tensile strength at break measured based on JIS K6251 is 2.0        or less MPa, and    -   (2) tensile elongation at break EB (%) of a resin composition        obtained satisfies the following expression of relations        (expression 1) and (expression 2), when blended with a        polypropylene derived resin that has 20 degree C. xylene        solluble component not more than 20 wt %.        R[3/5]−R[2/6]≧0.15  (expression 1)        S[2/6]≧−800  (expression 2)    -   (R[3/5] and R[2/6] are obtained by the following methods: a        curve is obtained by plotting tensile elongation at break EB (%)        (based on JIS K6251) of resin composition is taken as vertical        axis, and weight part rate Pa of a content of an olefin derived        copolymer contained in a resin composition is taken as        horizontal axis; a multiple regression curve in section regions        of Pa=0.30-0.50 and Pa=0.20-0.60 (Pa represents a content weight        percentage of an olefin derived copolymer contained in a resin        composition) of a multiple regression expression obtained by        quintic multiple regression of the curve is obtained; R[3/5] and        R[2/6] are defined as multiple correlation coefficients of a        primary straight line obtained by approximating of the multiple        regression curve by method of least squares. S[2/6] represents a        gradient of a primary straight line (expression) obtained by        approximating the above-mentioned multiple regression curve by a        method of least squares in section region of Pa=0.20-0.60. In        addition, in the above-mentioned multiple regression expression,        it is indispensable that data at least seven points Pa=0.00,        0.20, 0.30. 0.40, 0.50, 0.60 and 0.70 are contained.        Furthermore, when data at points of number beyond above case are        contained, it is indispensable that total Pa values exist at        0.10 or less of fixed interval mutually.

Among the above-mentioned olefin derived copolymers, in the light of thebelow-mentioned viewpoint, a tensile strength at break of the olefinderived copolymers of the present invention measured based on JIS K6251is 2.0 or less MPa, preferably 1.8 or less MPa, more preferably 1.6 orless MPa, still more preferably 1.4 or less MPa, further preferably 1.2or less MPa, furthermore preferably 1.0 or less MPa, most preferably 0.8or less MPa. If the value is out of this range, flexibility,transparency, resistance to whitening, and scratch resistance of thethermoplastic resin compositions obtained and the molded body containingthe thermoplastic resin compositions obtained will be decreased, and abalance of flexibility, heat resistance, and weather resistance willalso be impaired.

Furthermore, in the light of the same below-mentioned description inexpression (1),R[3/5]−R[2/6]≧0.15,preferably R[3/5]−R[2/6]≧0.20,more preferably R[3/5]−R[2/6]≧0.25,still more preferably R[3/5]−R[2/6]≧0.30,further preferably R[3/5]−R[2/6]≧0.35,most preferably R[3/5]−R[2/6]≧0.40.

Furthermore, in the light of the same below-mentioned description inexpression (2),S[2/6]≧−800,preferably, S[2/6]≧200, more preferably S[2/6]≧100,still more preferably S[2/6]≧50.

When an olefin derived copolymers of the present invention do notsatisfy a relationship of (expression 2), flexibility, transparency,resistance to whitening, scratch resistance, and tensile elongationcharacteristics of a thermoplastic resin compositions obtained and amolded body containing the thermoplastic resin compositions obtained aredecreased, and aba lance of flexibility, heat resistance, and weatherresistance is also decreased. Furthermore, when the olefin derivedcopolymer does not satisfy a relationship of (expression 1) and(expression 2), the surface character stability of the thermoplasticresin compositions obtained and of the molded body containing thethermoplastic resin compositions obtained is decreased.

In addition, a multiple regression expression, obtained by quinticmultiple regression of a curve that is obtained by plotting tensileelongation at break EB (%) (based on JIS K6251) of resin compositionstaken as vertical axis, and weight part rate Pa of a content of anolefin derived copolymers contained in resin compositions taken ashorizontal axis, is preferably calculated using data in each compositionblend point of 0.00, 0.20, 0.30, 0.40, 0.50, 0.60, and 0.70 of contentweight percentage Pa of olefin derived copolymer.

Specimen is molded into No. 3 dumbbell type form, and an tensileelongation at break EB (%) obtained based on JIS K6251 of a resincomposition is measured at elongation velocity of elongation velocity200 mm/min. Moreover, the number of specimens may be three pieces, andan arithmetic mean value may be used as a measurement result. However,in order to obtain measurement results with higher accuracy, the numberof specimens is preferably five or more, and more preferably seven ormore, and still more preferably 9 or more, and arithmetic mean value ofacquired tensile elongation at break value may be used as a result.Moreover, in order to eliminate results of cutting in irregular lowelongation it is preferable that results having 80% or less of tensileelongation at break of median of measurement result, or average of twopieces which faces across center are eliminated, and an arithmetic meanvalue of the remaining measurement results is used as a result.

Moreover, a blending with an olefin derived copolymer and apolypropylene derived resin that has not more than 20 wt % of 20 degreeC. xylene soluble component is performed by kneading each componentusing usual kneading equipment, for example, rubber mill, Brabendermixer, Banbury mixer, pressurized kneader, ruder, biaxial extruder, etc.Kneading temperature is a temperature at which all the mixed componentsare melted, and is usually set at 160-250 degrees C., and is preferablyset at 180-240 degrees C. Obtained resin composition is molded underpressure into a sample with predetermined thickness by a method based onJIS K6758 and is used as a sample for tensile test.

In addition, the above-mentioned quintic multiple regression expressionmay be calculated using, for example, a method represented in“Statistical Method for Chemist and Chemical Engineer (second edition)”(issued by Tokyo Kagaku Dojin Co., Ltd.) 6-3 and 6-4. Moreover, amultiple correlation coefficient R and gradient S which are acquired bystraight line regression using a method of least squares are calculatedby method represented in “Statistical Method for Chemist and ChemicalEngineer (second edition)” (issued by Tokyo Kagaku Dojin Co., Ltd.) 6-3and 6-4.

In olefin derived copolymers of the present invention, it is still morepreferable to satisfy the following (expression 3) relationship inaddition to the above-mentioned relationship also from the viewpoint ofa surface character stability of resin compositions.S[3/5]−S[2/6]≦50  (expression 3)

(S[3/5] and S[2/6] are obtained by the following methods: a curve isobtained by plotting tensile elongation at break EB (%) (based on JISK6251) of resin composition is taken as vertical axis, and weight partrate Pa of a content of an olefin derived copolymer contained in a resincomposition is taken as horizontal axis; a multiple regression curve insection regions of Pa=0.30-0.50 and Pa =0.20-0.60 (Pa represents contentweight percentage of an olefin derived copolymer contained in a resincomposition) of a multiple regression expression obtained by quinticmultiple regression of the curve is obtained; S[3/5] and S[2/6]represents a gradient of a primary straight line (expression) obtainedby approximating the above-mentioned multiple regression curve by amethod of least squares.)

In this relationship,preferably S[3/5]−S[2/6]≦−70,more preferably S[3/5]−S[2/6]≦−90,especially preferably S[3/5]−S[2/6]≦−110,most preferably S[3/5]−S[2/6]≦−120.

When olefin derived copolymers of the present invention do not satisfy arelationships of (expression 2) and (expression 3), the surfacecharacter stability of the thermoplastic resin compositions obtained andof the molded body containing the thermoplastic resin compositionsobtained may sometimes be decreased.

In addition, a polypropylene derived resin (X) in polypropylene derivedresins with 20-degree C. xylene soluble component of not more than 20 wt%, indicated by (2) of the present invention, represents a polypropylenederived resin that is chosen from polypropylene derived resins describedin full detail (i-4) in the below paragraph and that satisfies followingrequirements described below. In addition, 20-degree C. xylene solublecomponent of a polypropylene derived resin is a value according to thefollowing method and conditions. That is, polypropylene derived resinabout 200 mg is weighed, and it is mixed with xylene 10 ml, and inboiling xylene, dissolved for 50 minutes. After predetermined period,cooled for 20 minutes at room temperature, the polypropylene derivedresin is crystallized in 0-degree C. iced water. Then, the solution iskept in a 20-degree C. homothermal water bath for 1 hour. Subsequently,a xylene soluble component and a xylene non-soluble component areseparated by filtering, and the xylene non-soluble component is drieduntil it reaches constant weight in a vacuum dryer. After the xylenenon-soluble component is weighed, and a weight difference from theoriginal sample was obtained as a weight of xylene soluble component.Xylene soluble component (wt %) is obtained as a percentage of a xylenesoluble component weight to an original sample weight.

Moreover, it is preferable that a crystallization temperature Tc (degreeC.) and crystallization calorie ΔH (mj/mg) measured using a differentialscanning calorimeter (DSC) of a polypropylene derived resin (X) with20-degree C. xylene soluble component of not more than 20 wt % maysatisfy the following relationship. (in addition in measuring DSC, ameasurement is performed in both of the process of rising temperatureand constant temperature at the rate of 10 degrees C./min using, forexample, DSC220C (apparatus by SEIKO Electronic Ind., Co.) based on JISK7121 and JIS K7122.)

 −10≦[ΔH−(Tc×1.4)−62]≦10,more preferably −8≦[ΔH−(Tc×1.4)−62]≦8,still preferably −6≦[ΔH−(Tc×1.4)−62]≦6.

If a polypropylene derived resin (X) with 20-degree C. xylene solublecomponent of not more than 20 wt % goes out of this range, a specificolefin derived copolymer may not be judged correctly that can provide athermoplastic resin composition having outstanding flexibility,transparency, resistance to whitening, scratch resistance, elongationand surface stability characteristics.

Next, a polypropylene derived resin (X) with 20-degree C. xylene solublecomponent of not more than 20 wt % is a crystalline polypropylene thatmainly has an isotactic or syndiotactic sequence structure, andpreferably homogenous type and random type containing comonomer, morepreferably random type polypropylene derived resin containing comonomer.In addition, in manufacturing the polypropylene derived resin, vaporphase polymerization method, bulk polymerization method, and solventpolymerization method may be adopted. And there is especially nolimitation for a number average molecular weight of polymer, and ispreferably adjusted to 10000-1000000.

As a method of manufacturing polypropylene derived resin (X) which has20-degree C. xylene soluble component not more than 20 wt %, generally,following methods may be mentioned: a method wherein, homopolymerizedpropylene is obtained using Ziegler-Natta type catalyst in whichso-called solid transition metal components containing titanium, andorganic metal components are used in combination or a metallocenecatalyst that comprises transition metal compounds of the 4th to 6thgroup in periodic table with at least one cyclopentadienyl frame andco-catalyst components by slurry polymerization, vapor phasepolymerization, and bulk polymerization; and a method wherein,copolymerized propylene is obtained by copolymerising propylene and oneor more kinds of olefins chosen from olefin with 2-12 carbons other thanpropylene. In addition, it is also possible to use commerciallyavailable corresponding materials.

Next, in the light of flexibility of blended materials with polyolefinresins it is preferable that olefin derived copolymers of the presentinvention satisfy the following characteristics in addition to theabove-mentioned characteristics. That is, flexural modulus (Ua (MPa)) ofa thermoplastic resin compositions obtained as blended materials withhomogeneous polypropylene resin measured based on JIS K7203 preferablysatisfies a relationship of the following expression,Ua≦1.5×Sa×(Ta/100)^(3.3),more preferably Ua≦1.4×Sa×(Ta/100)^(3.3),still more preferably Ua≦1.3×Sa×(Ta/100)^(3.3),especially preferably Ua≦1.2×Sa×(Ta/100)^(3.3).

If Ua goes out of the above-mentioned range, flexibility, transparency,resistance to whitening, and scratch resistance of the thermoplasticresin compositions obtained and a molded body containing thethermoplastic resin compositions obtained may be decreased. In addition,in the above-mentioned expression, Sa represents flexural modulus (MPa)of the homogeneous polypropylene resins used for blending, measuredbased on JIS K7203, and Ta represents added weight part (wt %) of thehomogeneous polypropylene resins in the thermoplastic resincompositions.

Next, an intrinsic viscosity [η] of an olefin derived copolymer of thepresent invention in tetralin solvent at temperature of 135 degrees C.is preferably 0.3-10.0, more preferably 0.5-7.0, and still morepreferably 0.7-5.0. If the intrinsic viscosity is too low, scratchresistance and surface character stability of a molded body containingthermoplastic resin compositions obtained and a thermoplastic resincompositions obtained may be decreased. Moreover, if the intrinsicviscosity is too high, flexibility and transparency of a molded bodycontaining the thermoplastic resin compositions obtained and thethermoplastic resin compositions obtained may be decreased.

Measurement of intrinsic viscosity [η] is performed using an Ubbelohdeviscometer in 135-degree C. tetralin. Sample 300 mg is dissolved in 100ml tetralin, and 3 mg/ml solution was prepared. Furthermore, thesolution concerned is diluted into 1/2, 1/3, and 1/5, and a viscosity ofeach diluted solution is measured in 135 degrees C. (±0.1 degrees C.)oil thermostat. In each concentration, measurement is repeated 3 timesand an averaged value is adopted.

A molecular weight distribution (Mw/Mn) of an olefin derived copolymersof the present invention, measured by gel permeation chromatography(GPC) is preferably five or less, more preferably four or less, andstill more preferably three or less. When a molecular weightdistribution is too wide, flexibility of a molded body containingthermoplastic resin compositions obtained and a thermoplastic resincompositions obtained may be inferior. And moreover, that a molecularweight distribution of a polymer obtained by one-bath polymerization islarge generally means a wide intermolecular composition distribution. Insuch a case, decrease in surface character with the passage of time of athermoplastic resin compositions obtained and a molded body containingthe thermoplastic resin compositions may be observed.

As for molecular weight distribution, measurement is performed by gelpermeation chromatography (GPC) method (for example, 150 C/GPCequipment, apparatus made by Waters Co., Ltd.) Measurement conditionsare as follows; elution temperature: 140 degrees C.; column used: forexample, Sodex Packed Column A-80M (by Showa Denko K.K.); molecularweight standard substance: polystyrene (for example, made by TOSOHCORP., molecular weight 68-8400000). From obtained polystyrene convertedweight average molecular weight (Mw) and number average molecular weight(Mn), ratio (Mw/Mn) is calculated and this is defined as a molecularweight distribution. A measuring sample of about five mg polymer isdissolved in five ml o-dichlorobenzene, and solution with aconcentration of about one mg/ml is obtained. Obtained sample solution400 micro litter is injected, detection is performed using a refractiveindex detecting element at elution solvent flow velocity of 1.0 ml/min.

Next, when measurement is performed based on JIS K7122 usingdifferential scanning calorimeter (DSC), an olefin derived copolymer ofthe present invention preferably has neither a peak of one or more J/gbased on fusion of crystal nor a peak of one or more J/g based oncrystallization. When it has the peaks, flexibility, transparency,resistance to whitening, and scratch resistance of a molded bodycontaining thermoplastic resin compositions obtained and a thermoplasticresin compositions obtained may be decreased.

Furthermore in detail, a glass transition temperature of olefin derivedcopolymers of the present invention (Tg) is preferably −10 degrees C. orlower, more preferably −20 degrees C. or lower, and still morepreferably −25 degrees C. or lower.

As a differential scanning calorimeter, DSC220C by SEIKO ElectronicInd., Co. is used, and a measurement is performed in both of temperaturerising and temperature fall process at the rate of 10 degrees C./min.

Next, although an olefin derived copolymer of the present invention maybe manufactured using well-known Ziegler-Natta type catalysts orwell-known single site catalysts (metallocene derived etc.), well-knownsingle site catalysts (metallocene derived etc.) are preferable in thelight of homogeneity of a composition distribution of the polymerobtained. As examples of the single site catalysts, for example,metallocene derived catalysts indicated in JP,58-19309,A, JP,60-35005,A,JP,60-35006,A, JP,60-35007,A, JP,60-35008,A, JP,61-130314,A,JP,3-163088,A, JP,4-268307,A, JP,9-12790,A, JP,9-87313,A,JP,10-508055,A, JP,11-80233,A, JP Kohyo No.10-508055, etc., andnon-metallocene derived complex catalysts given in JP,10-316710,A,JP,11-100394,A, JP,11-80228,A, JP,11-80227,A, JP Kohyo No.10-513489,JP,10-338706,A, and JP Kohyo No.11-71420 may be mentioned. Also amongthese, generally metallocene catalysts are used and furthermore, assuitable example of metallocene catalyst, a complex is preferable thathas at least one cyclopentadiene form anionic frame, and in the light offlexibility of polymers obtained a complex of transition metal of thethird group to the 12th group of periodic table that has C₁ symmetricalstructure. Furthermore, as an example of suitable manufacturing methodin which metallocene catalyst is used to obtain high molecule polymer, amethod of copolymerising two or more kinds of monomer components chosenfrom ethylene, propylene, α-olefin with 4-20 carbons, polyene compound,cyclic olefin, and vinyl aromatic compound in the presence of catalystsfor olefin polymerization in which following (α), and following (β)and/or following (γ) are used may be mentioned.

-   -   (α): at least one of transition metal complexes represented by        following general formulas [I]-[III],    -   (In the above-mentioned general formula [I]-[III] , M¹        represents a transition metal atom of a 4th group of periodic        table of element, and A represents atom of a 16th group of        periodic table of element, and J represents atom of a 14th group        of periodic table of element, respectively. Cp¹ represents a        group that has a cyclopentadiene form anion frame. X¹, X², R¹,        R², R³, R⁴, R⁵, and R⁶ represent independently hydrogen atom,        halogen atom, alkyl group, aralkyl group, aryl group,        substituted silyl group, alkoxy group, aralkyloxy group, aryloxy        group, or di-substituted amino group, respectively. X³        represents atom of the 16th group of periodic table of element.        R¹, R², R³, R⁴, R⁵, and R⁶ may bond together arbitrarily to form        rings. Two members selected for a group of M¹, A and J, Cp¹, X¹,        X², X³, R¹, R², R³, R⁴, R⁵, and R⁶ may be the same, or they may        be different from each other respectively.    -   (β): one or more kinds of aluminum compounds chosen from        following (β1)-(β3)    -   (β1) organic aluminum compound represented by a general formula        E¹ ₃AlZ_(3-a)    -   (β2) cyclic aluminoxane that has a structure represented by a        general formula {—Al(E²)—O—}_(b)    -   (β3) Linear aluminoxane that has a structure represented by a        general formula E³{—Al(E³)—O—}_(c)AlE³ ₂    -   (where, E¹, E², and E³ is hydrocarbon group, respectively, all        E, all E², and all E³ may be the same, or they may be different        from each other. Z represents hydrogen atom or halogen atom, and        all Z may be the same, or they may be different from each other.        Character a represents an integer satisfying 0<a≦3, b represents        an integer of two or more, and c represents an integer of one or        more.)    -   (γ): a boron compound selected from the following (γ1)-(γ3)    -   (γ1) a boron compound represented by a general formula BQ¹Q²Q³,    -   (γ2) a boron compound represented by a general formula        G⁺(BQ¹Q²Q³Q⁴)    -   (γ3) a boron compound represented by a general formula        (L—H)⁺(BQ¹Q²Q³Q⁴)    -   (where, B represents a boron atom of trivalent valence state, Q¹        to Q⁴ represents halogen atom, hydrocarbon group, halogenated        hydrocarbon group, substituted silyl group, alkoxy group, or        di-substituted amino group, and they may the same, or they maybe        different from each other. G⁺ represents inorganic or organic        cation, L represents neutral Lewis base, (L—H)⁺ represents        Broensted acid.)

Hereafter, detail description will be given.

(α) Transition metal complex will be described in this paragraph.Transition metal complex (α) is represented by a general formula [I],[II], or [III]. In general formulas [I], [II], or [III], a transitionmetal atom shown as M↑1 represents a transition metal element of the 4thgroup in periodic table of element (IUPAC Inorganic ChemistryNomenclature revised edition 1989), and, for example, titanium atom,zirconium atom, hafnium atom, etc. may be mentioned. It preferablyrepresents titanium atom or zirconium atom.

In general formulas [I], [II], or [III], as an atom of a 16th group ofperiodic table that represents element represented as A, for example,oxygen atom, sulfur atom, selenium atom, etc. may be mentioned andpreferably oxygen atom may be mentioned.

In general formula [I], [II], or [III], as an atom of a 14th group ofperiodic table that represents element represented as J, carbon atom,silicon atom, germanium atom, etc. may be mentioned, for example, andpreferably carbon atom or silicon atom may be mentioned.

As a group that is represented as substituent Cp¹ and hascyclopentadiene form anion frame, for example, η⁵-(substituted)cyclopentadienyl group, η⁵-(substituted) indenyl group, η⁵-(substituted)fluorenyl group, etc. may be mentioned. Specifically, for example,following groups may be mentioned; η⁵-cyclopentadienyl group, η⁵-methylcyclopentadienyl group, η⁵-dimethyl cyclopentadienyl group, η⁵-trimethylcyclopentadienyl group, η⁵-tetramethyl cyclopentadienyl group, η⁵-ethylcyclopentadienyl group, η⁵-n-propyl cyclopentadienyl group, η⁵-isopropyl cyclopentadienyl group, η⁵-n-butyl cyclopentadienyl group,η⁵-sec-butyl cyclopentadienyl group, η⁵-tert-butyl cyclopentadienylgroup, η⁵-n-pentyl cyclopentadienyl group. η⁵-neopentyl cyclopentadienylgroup, η⁵-n-hexyl cyclopentadienyl group, η⁵-n-octyl cyclopentadienylgroup, η⁵-phenyl cyclopentadienyl group, η⁵-naphthyl cyclopentadienylgroup, η⁵-trimethyl silyl cyclopentadienyl group, η⁵-triethyl silylcyclopentadienyl group, η⁵-tert-butyl dimethyl silyl cyclopentadienylgroup, η⁵-indenyl group, η⁵-methyl indenyl group, η⁵-dimethyl indenylgroup, η⁵-ethyl indenyl group, η⁵-n-propyl indenyl group, η⁵-isopropylindenyl group, η⁵-n-butyl indenyl group, η⁵-sec-butyl indenyl group,η⁵-tert-butyl indenyl group, η⁵-n-pentyl indenyl group, η⁵-neo pentylindenyl group, η⁵-n-hexyl indenyl group, η⁵-octyl indenyl group,η⁵-n-decyl indenyl group, η⁵-phenyl indenyl group, η⁵-methylphenylindenyl group, η⁵-naphthyl indenyl group, η⁵-trimethyl silyl indenylgroup, η⁵-triethyl silyl indenyl group, η⁵-tert-butyl dimethyl silylindenyl group, η⁵-tetrahydro indenyl group, η⁵-fluorenyl group,η⁵-methyl fluorenyl group, η⁵-dimethyl fluorenyl group, η⁵-ethylfluorenyl group, η⁵-diethyl fluorenyl group, η⁵-n-propyl fluorenylgroup, η⁵-di-n-propyl fluorenyl group, η⁵-iso propyl fluorenyl group,η⁵-diisopropyl fluorenyl group, η⁵-butyl fluorenyl group, η⁵-sec-butylfluorenyl group, η⁵-tert-butyl fluorenyl group, η⁵-di-n-butyl fluorenylgroup, η⁵-di-sec-butyl fluorenyl group, η⁵-di-tert-butyl fluorenylgroup, η⁵-n-pentyl fluorenyl group, η⁵-neo pentyl fluorenyl group,η⁵-n-hexyl fluorenyl group, η⁵-n-octyl fluorenyl group, η⁵-n-decylfluorenyl group, η⁵-n-dodecyl fluorenyl group, η⁵-phenyl fluorenylgroup, η⁵-di-phenyl fluorenyl group, η⁵-methyl phenyl fluorenyl group,η⁵-naphthyl fluorenyl group, η⁵-trimethyl silyl fluorenyl group,η⁵-bis-trimethyl silyl fluorenyl group, η⁵-triethyl silyl fluorenylgroup, η⁵-tert-butyl dimethyl silyl fluorenyl group, etc. Preferably,η⁵-cyclopentadienyl group, η⁵-methyl cyclopentadienyl group,η⁵-tert-butyl cyclopentadienyl group, η⁵-tetramethyl cyclopentadienylgroup, η⁵-indenyl group, or η⁵-fluorenyl group may be mentioned.

As halogen atom in substituents X¹, X², R¹, R², R³, R⁴, R⁵, and R⁶,fluorine atom, chlorine atom, bromine atom, iodine atom, etc. arementioned, and preferably chlorine atom or bromine atom, more preferablychlorine atom may be mentioned.

As alkyl group in substituents X¹, X², R¹, R², R³, R⁴, R⁵, and R⁶, alkylgroup with 1-20 carbon atoms is preferable, for example, methyl group,ethyl group, n-propyl group, isopropyl group, n-butyl group, sec-butylgroup, tert-butyl group, n-pentyl group, neo pentyl group, amyl group,n-hexyl group, n-octyl group, n-decyl group, n-dodecyl group,n-pentadecyl group, n-eicosyl group, etc. are mentioned, and morepreferably methyl group, ethyl group, iso propyl group, tert-butylgroup, or amyl group may be mentioned.

Each of these alkyl groups may be substituted by halogen atoms, such asfluorine atom, chlorine atom, bromine atom, and iodine atom. As alkylgroups with 1-20 carbon atoms substituted by halogen atoms, for example,fluoro methyl group, difluoro methyl group, trifluoro methyl group,chloro methyl group, dichloro methyl group, trichloro methyl group,bromo methyl group, dibromo methyl group, tribromo methyl group, iodomethyl group, diiodo methyl group, trilodo methyl group, fluoro ethylgroup, difluoro ethyl group, trifluoro ethyl group, tetrafluoro ethylgroup, pentafluoro ethyl group, chloro ethyl group, dichloro ethylgroup, trichloro ethyl group, tetrachloro ethyl group, pentachloro ethylgroup, bromo ethyl group, dibromo ethyl group, tribromo ethyl group,tetra bromo ethyl group, penta bromo ethyl group, perfluoro propylgroup, perfluoro butyl group, perfluoro pentyl group, perfluoro hexylgroup, perfluoro octyl group, perfluoro dodecyl group, perfluoro pentadecyl group, perfluoro eicosyl group, perchloro propyl group, perchlorobutyl group, perchloro pentyl group, perchloro hexyl group, perchlorooctyl group, perchloro dodecyl group, perchloro pentadecyl group,perchloro eicosyl group, perbromo propyl group, perbromo butyl group,perbromo pentyl group, perbromo hexyl group, perbromo octyl group,perbromo dodecyl group, perbromo pentadecyl group, perbromo eicosylgroup, etc. may be mentioned.

Moreover, each of these alkyl groups may be substituted partially byalkoxy groups, such as methoxy group and ethoxy group; aryloxy groups,such as phenoxy group; or aralkyl oxy groups, such as benzyloxy group.

As aralkyl groups in substituents X¹, X², R¹, R², R³, R⁴, R⁵, and R⁶,aralkyl groups with 7-20 carbon atoms are preferable, for example,benzyl group, (2-methyl phenyl)methyl group, (3-methyl phenyl)methylgroup, (4-methyl phenyl)methyl group, (2,3-dimethyl phenyl)methyl group,(2,4-dimethyl phenyl)methyl group, (2,5-dimethyl phenyl)methyl group,(2,6-dimethyl phenyl)methyl group, (3,4-dimethyl phenyl)methyl group,(4,6-dimethyl phenyl)methyl group, (2,3,4-trimethyl phenyl)methyl group,(2,3,5-trimethyl phenyl)methyl group, (2,3,6-trimethyl phenyl)methylgroup, (3,4,5-trimethyl phenyl)methyl group, (2,4,6-trimethylphenyl)methyl group, (2,3,4,5-tetramethyl phenyl)methyl group, methylgroup (2,3,4,6-tetramethylphenyl), methyl group (2,3,5,6-tetramethylphenyl), methyl group (penta methyl phenyl), methyl group (ethylphenyl), methyl group (n-propyl phenyl), methyl group (iso propylphenyl), methyl group (n-butylphenyl), (2,3,4,6-tetramethylphenyl)methyl group, (2,3,5,6-tetramethylphenyl)methyl group, (pentamethyl phenyl)methyl group, (Ethyl phenyl)methyl group, (n-propylphenyl)methyl group, (iso-propyl phenyl)methyl group,(n-butylphenyl)methyl group, (sec-butylphenyl)methyl group,(tert-butylphenyl)methyl group, (n-pentyl phenyl)methyl group, (neopentyl phenyl)methyl group, (n-hexyl phenyl)methyl group, (n-octylphenyl)methyl group, (n-decyl phenyl)methyl group, (n-dodecylphenyl)methyl group, (n-tetrapod decyl phenyl)methyl group, naphthylmethyl group, anthracenyl methyl group, etc. may be mentioned, and morepreferably benzyl group is mentioned.

Each of these aralkyl groups may be substituted partially by halogenatoms, such as fluorine atom, chlorine atom, bromine atom, and iodineatom; alkoxy groups, such as methoxy group and ethoxy group; aryloxygroups, such as phenoxy group; or aralkyl oxy groups, such as benzyloxygroup.

As substituents X¹, X², R¹, R², R³, R⁴, R⁵, and R⁶, aryl groups with6-20 carbon atoms is preferable, for example, phenyl group, 2-trillgroup, 3-trill group, 4-trill group, 2,3-xylyl group, 2,4-xylyl group,2,5-xylyl group, 2,6-xylyl group, 3,4-xylyl group, 3,5-xylyl group,2,3,4-trimethyl phenyl group, 2,3,5-trimethyl phenyl group,2,3,6-trimethyl phenyl group, 2,4,6-trimethyl phenyl group,3,4,5-trimethyl phenyl group, 2,3,4,5-tetramethyl phenyl group,2,3,4,6-tetramethyl phenyl group, 2,3,5,6-tetramethyl phenyl group,pentamethyl phenyl group, ethylphenyl group, n-propyl phenyl group,iso-propyl phenyl group, n-butylphenyl group, sec-butylphenyl group,tert-butylphenyl group, n-pentylphenyl group, neo-pentyl phenyl group,n-hexylphenyl group, n-octylphenyl group, n-decylphenyl group,n-dodecylphenyl group, n-tetradecyl phenyl group, naphthyl group,anthracenyl group, etc. may be mentioned, and more preferably phenylgroup is mentioned.

Each of these aryl groups may be partially substituted by halogen atoms,such as fluorine atom, chlorine atom, bromine atom, and iodine atom;alkoxy groups, such as methoxy group and ethoxy group; aryloxy groups,such as phenoxy group; or aralkyloxy groups, such as benzyl oxy group.

Substituted silyl groups in substituentd X¹, X², R¹, R², R³, R⁴, R⁵, andR⁶ represents silyl groups substituted by hydrocarbon group. Ashydrocarbon groups here, for example, alkyl group with 1-10 carbonatoms, such as methyl group, ethyl group, n-propyl group, iso-propylgroup, n-butyl group, sec-butyl group, tert-butyl group, iso-butylgroup, n-pentyl group, n-hexyl group, and cyclohexyl group; aryl groups,such as phenyl group, etc. may be mentioned. As these substituted silylgroups with 1-20 carbon atoms, for example, mono-substituted silyl groupwith 1-20 carbon atoms, such as methyl silyl group, ethyl silyl group,and phenyl silyl group, and di-substituted silyl group with 2-20 carbonatoms, such as dimethyl silyl group, diethyl silyl group, and diphenylsilyl group, and tri-substituted silyl group with 3-20 carbon atoms.such as trimethyl silyl group, triethyl silyl group, tri-n-propyl silylgroup, tri-iso-propyl silyl group, tri-n-butyl silyl group,tri-sec-butyl silyl group, tri-tert-butyl silyl group, tri-iso-butylsilyl group, tert-butyl-dimethyl silyl group, tri-n-pentyl silyl group,tri-n-hexyl silyl group, tri-cyclohexyl silyl group, and triphenylsilylgroup, etc. may be mentioned, and preferably trimethyl silyl group,tert-butyl dimethyl silyl group, or triphenylsilyl group may bementioned.

Each hydrocarbon group of these substituting silyl groups may bepartially substituted by halogen atoms, such as fluorine atom, chlorineatom, bromine atom, and iodine atom; alkoxy groups, such as methoxygroup and ethoxy group; aryloxy groups, such as phenoxy group; oraralkyl oxy groups, such as benzyl oxy group.

As alkoxy groups in substituents X¹, X², R¹, R², R³, R⁴, R⁵, and R⁶,alkoxy groups with 1-20 carbon atoms are preferable, for example,methoxy group, ethoxy group, n-propoxy group, iso-propoxy group,n-butoxy group, sec-butoxy group, tert-butoxy group, n-pentoxy group,neopentoxy group, n-hexoxy group, n-octoxy group, n-dodecoxy group,n-pentadecoxy group, n-icosaoxy group, etc. may be mentioned, and morepreferably, methoxy group, ethoxy group, or tert-butoxy group may bementioned.

Each of these alkoxy groups may be partially substituted by halogenatoms, such as fluorine atom, chlorine atom, bromine atom, and iodineatom; alkoxy groups, such as methoxy group and ethoxy group; aryloxygroups, such as phenoxy group; or aralkyl oxy groups, such as benzyl oxygroup.

As aralkyl oxy groups in substituents X¹, X², R¹, R², R³, R⁴, R⁵, or R⁶,aralkyl oxy groups with 7-20 carbon atoms is preferable, for example,benzyl oxy group, (2-methyl phenyl)methoxy group, (3-methylphenyl)methoxy group, (4-methyl phenyl)methoxy group, (2,3-dimethylphenyl)methoxy group, (2,4-dimethyl phenyl)methoxy group, (2,5-dimethylphenyl)methoxy group, (2,6-dimethyl phenyl)methoxy group,(3,4-dimethylphenyl)methoxy group, (3,5-dimethylphenyl)methoxy group,(2,3,4-trimethyl phenyl)methoxy group, (2,3,5-trimethyl phenyl)methoxygroup, (2,3,6-trimethyl phenyl)methoxy group, (2,4,5-trimethylphenyl)methoxy group, (2,4,6-trimethyl phenyl)methoxy group,(3,4,5-trimethyl phenyl)methoxy group, (2,3,4,5-tetramethylphenyl)methoxy group, (2,3,4,6-tetramethyl phenyl)methoxy group,(2,3,5,6-tetramethyl phenyl)methoxy group, (Penta methyl phenyl)methoxygroup, (Ethyl phenyl)methoxy group, (n-propyl phenyl)methoxy group, (isopropyl phenyl)methoxy group, (n-butylphenyl)methoxy group,(sec-butylphenyl)methoxy group, (tert-butylphenyl)methoxy group,(n-hexylphenyl)methoxy group, (n-octyl phenyl)methoxy group, (n-decylphenyl)methoxy group, (n-tetrapod decyl phenyl)methoxy group, naphthylmethoxy group, anthracenyl methoxy group, etc. may be mentioned, andmore preferably benzyl oxy group may be mentioned.

Each of these aralkyl oxy groups may be partially substituted by halogenatoms, such as fluorine atom, chlorine atom, bromine atom, and iodineatom; alkoxy groups, such as methoxy group and ethoxy group; aryloxygroups, such as phenoxy group; or aralkyl oxy groups, such as benzyl oxygroup.

As an aryloxy groups in substituents X¹, X², R¹, R², R³, R⁴, R⁵, and R⁶,aryloxy group with 6-20 carbon atoms is preferable, for example, phenoxygroup, 2-methyl phenoxy group, 3-methyl phenoxy group, 4-methyl phenoxygroup, 2,3-dimethyl phenoxy group, 2,4-dimethyl phenoxy group,2,5-dimethyl phenoxy group, 2,6-dimethyl phenoxy group, 3,4-dimethylphenoxy group, 3,5-dimethyl phenoxy group, 2,3,4-trimethyl phenoxygroup, 2,3,5-trimethyl phenoxy group, 2,3,6-trimethyl phenoxy group,2,4,5-trimethyl phenoxy group, 2,4,6-trimethyl phenoxy group,3,4,5-trimethyl phenoxy group, 2,3,4,5-tetramethyl phenoxy group,2,3,4,6-tetramethyl phenoxy group, 2,3,5,6-tetramethyl phenoxy group,penta methyl phenoxy group, ethyl phenoxy group, n-propyl phenoxy group,iso-propyl phenoxy group, n-butyl phenoxy group, sec-butyl phenoxygroup, tert-butyl phenoxy group, n-hexyl phenoxy group, n-octyl phenoxygroup, n-decyl phenoxy group, n-tetradecyl phenoxy group, naphthoxygroup, anthracenoxy group, etc. may be mentioned.

Each of these aryloxy groups may be partially substituted by halogenatoms, such as fluorine atom, chlorine atom, bromine atom, and iodineatom; alkoxy groups, such as methoxy group and ethoxy group; aryloxygroups, such as phenoxy group; or aralkyl oxy groups, such as benzyl oxygroup.

Di-substituted amino groups in substituents X¹, X², R¹, R², R³, R⁴, R⁵,and R⁶ represents amino group substituted by two hydrocarbon groups.Here as hydrocarbon groups, for example, alkyl groups with 1-10 carbonatoms, such as methyl group, ethyl group, n-propyl group, iso-propylgroup, n-butyl group, sec-butyl group, tert-butyl group, isobutyl group,n-pentyl group, n-hexyl group, and cyclo hexyl group; and aryl groupswith 6-10 carbon atoms, such as phenyl group; aralkyl group with 7-10carbon atoms, etc. may be mentioned. As di-substituted amino groupsubstituted by hydrocarbon group with these 1-10 carbon atoms, forexample, dimethyl amino group, diethyl amino group, di-n-propyl aminogroup, diiso-propyl amino group, di-n-butyl amino group, di-sec-butylamino group, di-tert-butyl amino group, di-iso-butyl amino group,tert-butyl iso-propyl amino group, di-n-hexyl amino group, di-n-octylamino group, di-n-decyl amino group, diphenyl amino group, bis-trimethylsilyl amino group, bis-tert-butyl dimethyl silyl amino group, etc. maybe mentioned, and preferably dimethyl amino group or diethyl amino groupmay be mentioned. Each of these amino groups may be partiallysubstituted by halogen atoms, such as fluorine atom, chlorine atom,bromine atom, and iodine atom; alkoxy groups, such as methoxy group andethoxy group; aryloxy groups, such as phenoxy group; or aralkyl oxygroups, such as benzyl oxy group.

Substituents X¹, X², R¹, R², R³, R⁴, R⁵, and R⁶ may be bonded togetherarbitrarily to form rings.

As preferable R¹, alkyl group, aralkyl group, aryl group, andsubstituted silyl group may be mentioned. As preferable X¹ and X²,independently halogen atom, alkyl group, aralkyl group, alkoxy group,aryloxy group, and di-substituted amino group may be mentioned,respectively, and more preferably, halogen atom and alkoxy group may bementioned. As atoms of the 16th group of periodic table that representelement represented as X³ in general formula [II] or [III], for example,oxygen atom, sulfur atom, selenium atom, etc. may be mentioned andpreferably t represents oxygen atom.

As transition metal complex represented by general formula [1], forexample, following complex may be mentioned;methylene(cyclopentadienyl)(3,5-dimethyl-2-phenoxy)titanium dichloride,methylene(cyclopentadienyl)(3-tert-butyl-2-phenoxy)titanium dichloride,methylene(cyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titaniumdichloride, methylene(cyclopentadienyl)(3-phenyl-2-phenoxy)titaniumdichloride, methylene(cyclopentadienyl)(3-tert-butyl dimethylsilyl-5-methyl-2-phenoxy)titanium dichloride,methylene(cyclopentadienyl)(3-trimethylsilyl-5-methyl-2-phenoxy)titanium dichloride,methylene(cyclopentadienyl)(3-tert-butyl-5-methoxy-2-phenoxy)titaniumdichloride,methylene(cyclopentadienyl)(3-tert-butyl-5-chloro-2-phenoxy)titaniumdichloride, methylene(methylcyclopentadienyl)(3,5-dimethyl-2-phenoxy)titanium dichloride,methylene(methyl cyclopentadienyl)(3-tert-butyl-2-phenoxy) titaniumdichloride, methylene(methylcyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium dichloride,methylene(methyl cyclopentadienyl)(3-phenyl-2-phenoxy)titaniumdichloride, methylene(methyl cyclopentadienyl)(3-tert-butyl dimethylsilyl-5-methyl-2-phenoxy)titanium dichloride, methylene(methylcyclopentadienyl)(3-trimethyl silyl-5-methyl-2-phenoxy)titaniumdichloride, methylene(methylcyclopentadienyl)(3-tert-butyl-5-methoxy-2-phenoxy)titanium dichloride,methylene(methylcyclopentadienyl)(3-tert-butyl-5-chloro-2-phenoxy)titanium dichloride,methylene(tert-butyl cyclopentadienyl)(3,5-dimethyl-2-phenoxy)titaniumdichloride, methylene(tert-butylcyclopentadienyl)(3-tert-butyl-2-phenoxy)titanium dichloride,methylene(tert-butylcyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium dichloride,methylene(tert-butyl cyclopentadienyl)(3-phenyl-2-phenoxy)titaniumdichloride, methylene(tert-butyl cyclopentadienyl)(3-tert-butyl dimethylsilyl-5-methyl-2-phenoxy)titanium dichloride, methylene(tert-butylcyclopentadienyl)(3-trimethyl silyl-5-methyl-2-phenoxy)titaniumdichloride, methylene(tert-butylcyclopentadienyl)(3-tert-butyl-5-methoxy-2-phenoxy)titanium dichloride,methylene(tert-butylcyclopentadienyl)(3-tert-butyl-5-chloro-2-phenoxy)titanium dichloride,methylene(tetramethyl cyclopentadienyl)(3,5-dimethyl-2-phenoxy)titaniumdichloride, methylene(tetramethylcyclopentadienyl)(3-tert-butyl-2-phenoxy)titanium dichloride,methylene(tetramethylcyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium dichloride,methylene(tetramethyl cyclopentadienyl)(3-phenyl-2-phenoxy)titaniumdichloride, methylene(tetramethyl cyclopentadienyl)(3-tert-butyldimethyl silyl-5-methyl-2-phenoxy)titanium dichloride,methylene(tetramethyl cyclopentadienyl)(3-trimethylsilyl-5-methyl-2-phenoxy)titanium dichloride, methylene(tetramethylcyclopentadienyl)(3-tert-butyl-5-methoxy-2-phenoxy)titanium dichloride,methylene(tetramethylcyclopentadienyl)(3-tert-butyl-5-chloro-2-phenoxy)titanium dichloride,methylene(trimethyl silylcyclopentadienyl)(3,5-dimethyl-2-phenoxy)titanium dichloride,methylene(trimethyl silylcyclopentadienyl)(3-tert-butyl-2-phenoxy)titanium dichloride,methylene(trimethyl silylcyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium dichloride,methylene(trimethyl silyl cyclopentadienyl)(3-phenyl-2-phenoxy)titaniumdichloride, methylene(trimethyl silyl cyclopentadienyl)(3-tert-butyldimethyl silyl-5-methyl-2-phenoxy)titanium dichloride,methylene(trimethyl silyl cyclopentadienyl)(3-trimethylsilyl-5-methyl-2-phenoxy)titanium dichloride, methylene(trimethyl silylcyclopentadienyl)(3-tert-butyl-5-methoxy-2-phenoxy)titanium dichloride,methylene(trimethyl silylcyclopentadienyl)(3-tert-butyl-5-chloro-2-phenoxy)titanium dichloride;methylene(fluorenyl)(3,5-dimethyl-2-phenoxy)titanium dichloride,methylene (fluorenyl)(3-tert-butyl-2-phenoxy)titanium dichloride,methylene(fluorenyl)(3-tert-butyl-5-methyl-2-phenoxy)titaniumdichloride, methylene(fluorenyl)(3-phenyl-2-phenoxy)titanium dichloride,methylene(fluorenyl)(3-tert-butyl dimethylsilyl-5-methyl-2-phenoxy)titanium dichloride,methylene(fluorenyl)(3-trimethyl silyl-5-methyl-2-phenoxy)titaniumdichloride,methylene(fluorenyl)(3-tert-butyl-5-methoxy-2-phenoxy)titaniumdichloride,methylene(fluorenyl)(3-tert-butyl-5-chloro-2-phenoxy)titaniumdichloride,isopropylidene(cyclopentadienyl)(3,5-dimethyl-2-phenoxy)titaniumdichloride,isopropylidene(cyclopentadienyl)(3-tert-butyl-2-phenoxy)titaniumdichloride,isopropylidene(cyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titaniumdichloride, isopropylidene(cyclopentadienyl)(3-phenyl-2-phenoxy)titaniumdichloride, isopropylidene(cyclopentadienyl)(3-tert-butyl dimethylsilyl-5-methyl-2-phenoxy)titanium dichloride,isopropylidene(cyclopentadienyl)(3-trimethylsilyl-5-methyl-2-phenoxy)titanium dichloride,isopropylidene(cyclopentadienyl)(3-tert-butyl-5-methoxy-2-phenoxy)titaniumdichloride,isopropylidene(cyclopentadienyl)(3-tert-butyl-5-chloro-2-phenoxy)titaniumdichloride, isopropylidene(methylcyclopentadienyl)(3,5-dimethyl-2-phenoxy)titanium dichloride,isopropylidene(methyl cyclopentadienyl)(3-tert-butyl-2-phenoxy)titaniumdichloride, isopropylidene(methylcyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium dichloride,isopropylidene(methyl cyclopentadienyl)(3-phenyl-2-phenoxy)titaniumdichloride, isopropylidene(methyl cyclopentadienyl)(3-tert-butyldimethyl silyl-5-methyl-2-phenoxy)titanium dichloride,isopropylidene(methyl cyclopentadienyl)(3-trimethylsilyl-5-methyl-2-phenoxy)titanium dichloride, isopropylidene(methylcyclopentadienyl)(3-tert-butyl-5-methoxy-2-phenoxy)titanium dichloride,isopropylidene(methylcyclopentadienyl)(3-tert-butyl-5-chloro-2-phenoxy)titanium dichloride,isopropylidene(tert-butylcyclopentadienyl)(3,5-dimethyl-2-phenoxy)titanium dichloride,isopropylidene(tert-butylcyclopentadienyl)(3-tert-butyl-2-phenoxy)titanium dichloride,isopropylidene(tert-butylcyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium dichloride,isopropylidene(tert-butyl cyclopentadienyl)(3-phenyl-2-phenoxy)titaniumdichloride, isopropylidene(tert-butyl cyclopentadienyl)(3-tert-butyldimethyl silyl-5-methyl-2-phenoxy)titanium dichloride,isopropylidene(tert-butyl cyclopentadienyl)(3-trimethylsilyl-5-methyl-2-phenoxy)titanium dichloride, isopropylidene(tert-butylcyclopentadienyl)(3-tert-butyl-5-methoxy-2-phenoxy)titanium dichloride,isopropylidene(tert-butylcyclopentadienyl)(3-tert-butyl-5-chloro-2-phenoxy)titanium dichloride,isopropylidene(tetramethylcyclopentadienyl)(3,5-dimethyl-2-phenoxy)titanium dichloride,isopropylidene(tetramethylcyclopentadienyl)(3-tert-butyl-2-phenoxy)titanium dichloride,isopropylidene(tetramethylcyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium dichloride,isopropylidene(tetramethyl cyclopentadienyl)(3-phenyl-2-phenoxy)titaniumdichloride, isopropylidene(tetramethyl cyclopentadienyl)(3-tert-butyldimethyl silyl-5-methyl-2-phenoxy)titanium dichloride,isopropylidene(tetramethyl cyclopentadienyl)(3-trimethylsilyl-5-methyl-2-phenoxy)titanium dichloride, isopropylidene(tetramethylcyclopentadienyl)(3-tert-butyl-5-methoxy-2-phenoxy)titanium dichloride,isopropylidene(tetramethylcyclopentadienyl)(3-tert-butyl-5-chloro-2-phenoxy)titanium dichloride,isopropylidene(trimethyl silylcyclopentadienyl)(3,5-dimethyl-2-phenoxy)titanium dichloride,isopropylidene(trimethyl silylcyclopentadienyl)(3-tert-butyl-2-phenoxy)titanium dichloride,isopropylidene(trimethyl silylcyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium dichloride,isopropylidene(trimethyl silylcyclopentadienyl)(3-phenyl-2-phenoxy)titanium dichloride,isopropylidene(trimethyl silyl cyclopentadienyl)(3-tert-butyl dimethylsilyl-5-methyl-2-phenoxy)titanium dichloride, isopropylidene(trimethylsilyl cyclopentadienyl)(3-trimethyl silyl-5-methyl-2-phenoxy)titaniumdichloride, isopropylidene(trimethyl silylcyclopentadienyl)(3-tert-butyl-5-methoxy-2-phenoxy)titanium dichloride,isopropylidene(trimethyl silylcyclopentadienyl)(3-tert-butyl-5-chloro-2-phenoxy)titanium dichloride,isopropylidene(fluorenyl)(3,5-dimethyl-2-phenoxy)titanium dichloride,isopropylidene(fluorenyl)(3-tert-butyl-2-phenoxy)titanium dichloride,isopropylidene(fluorenyl)(3-tert-butyl-5-methyl-2-phenoxy)titaniumdichloride, isopropylidene(fluorenyl)(3-phenyl-2-phenoxy titaniumdichloride, isopropylidene(fluorenyl)(3-tert-butyl dimethylsilyl-5-methyl-2-phenoxy)titanium dichloride,isopropylidene(fluorenyl)(3-trimethyl silyl-5-methyl-2-phenoxy)titaniumdichloride,isopropylidene(fluorenyl)(3-tert-butyl-5-methoxy-2-phenoxy)titaniumdichloride,isopropylidene(fluorenyl)(3-tert-butyl-5-chloro-2-phenoxy)titaniumdichloride, diphenylmethylene(cyclopentadienyl)(3,5-dimethyl-2-phenoxy)titanium dichloride,diphenyl methylene(cyclopentadienyl)(3-tert-butyl-2-phenoxy)titaniumdichloride, diphenylmethylene(cyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titaniumdichloride, diphenylmethylene(cyclopentadienyl)(3-phenyl-2-phenoxy)titanium dichloride,diphenyl methylene(cyclopentadienyl)(3-tert-butyl dimethylsilyl-5-methyl-2-phenoxy)titanium dichloride, diphenylmethylene(cyclopentadienyl)(3-trimethylsilyl-5-methyl-2-phenoxy)titanium dichloride, diphenylmethylene(cyclopentadienyl)(3-tert-butyl-5-methoxy-2-phenoxy)titaniumdichloride, diphenylmethylene(cyclopentadienyl)(3-tert-butyl-5-chloro-2-phenoxy)titaniumdichloride, diphenyl methylene(methylcyclopentadienyl)(3,-dimethyl-2-phenoxy)titanium dichloride, diphenylmethylene(methyl cyclopentadienyl)(3-tert-butyl-2-phenoxy)titaniumdichloride, diphenyl methylene(methylcyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium dichloride,diphenyl methylene(methyl cyclopentadienyl)(3-phenyl-2-phenoxy)titaniumdichloride, diphenyl methylene(methyl cyclopentadienyl)(3-tert-butyldimethyl silyl-5-methyl-2-phenoxy)titanium dichloride, diphenylmethylene(methyl cyclopentadienyl)(3-trimethylsilyl-5-methyl-2-phenoxy)titanium dichloride, diphenyl methylene(methylcyclopentadienyl)(3-tert-butyl-5-methoxy-2-phenoxy)titanium dichloride,diphenyl methylene(methylcyclopentadienyl)(3-tert-butyl-5-chloro-2-phenoxy)titanium dichloride,diphenyl methylene(tert-butylcyclopentadienyl)(3,5-dimethyl-2-phenoxy)titanium dichloride, diphenylmethylene(tert-butyl cyclopentadienyl)(3-tert-butyl-2-phenoxy)titaniumdichloride, diphenyl methylene(tert-butylcyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium dichloride,diphenyl methylene(tert-butylcyclopentadienyl)(3-phenyl-2-phenoxy)titanium dichloride, diphenylmethylene(tert-butyl cyclopentadienyl (3-tert-butyl dimethylsilyl-5-methyl-2-phenoxy)titanium dichloride, diphenylmethylene(tert-butyl cyclopentadienyl)(3-trimethylsilyl-5-methyl-2-phenoxy)titanium dichloride, diphenylmethylene(tert-butylcyclopentadienyl)(3-tert-butyl-5-methoxy-2-phenoxy)titanium dichloride,diphenyl methylene(tert-butylcyclopentadienyl)(.3-tert-butyl-5-chloro-2-phenoxy)titanium dichloride,diphenyl methylene(tetramethylcyclopentadienyl)(3,5-dimethyl-2-phenoxy)titanium dichloride, diphenylmethylene(tetramethyl cyclopentadienyl)(3-tert-butyl-2-phenoxy)titaniumdichloride, diphenyl methylene(tetramethylcyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium dichloride,diphenyl methylene(tetramethylcyclopentadienyl)(3-phenyl-2-phenoxy)titanium dichloride, diphenylmethylene(tetramethyl cyclopentadienyl)(3-tert-butyl dimethylsilyl-5-methyl-2-phenoxy)titanium dichloride, diphenylmethylene(tetramethyl cyclopentadienyl)(3-trimethylsilyl-5-methyl-2-phenoxy titanium dichloride, diphenylmethylene(tetramethylcyclopentadienyl)(3-tert-butyl-5-methoxy-2-phenoxy)titanium dichloride,diphenyl methylene(tetramethylcyclopentadienyl)(3-tert-butyl-5-chloro-2-phenoxy)titanium dichloride,diphenyl methylene(trimethyl silylcyclopentadienyl)(3,5-dimethyl-2-phenoxy)titanium dichloride, diphenylmethylene(trimethyl silylcyclopentadienyl)(3-tert-butyl-2-phenoxy)titanium dichloride, diphenylmethylene(trimethyl silylcyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium dichloride,diphenyl methylene(trimethyl silylcyclopentadienyl)(3-phenyl-2-phenoxy)titanium dichloride, diphenylmethylene(trimethyl silyl cyclopentadienyl)(3-tert-butyl dimethylsilyl-5-methyl-2-phenoxy)titanium dichloride, diphenylmethylene(trimethyl silyl cyclopentadienyl)(3-trimethylsilyl-5-methyl-2-phenoxy)titanium, dichloride, diphenylmethylene(trimethyl silylcyclopentadienyl)(3-tert-butyl-5-methoxy-2-phenoxy)titanium dichloride,diphenyl methylene(trimethyl silylcyclopentadienyl)(3-tert-butyl-5-chloro-2-phenoxy)titanium dichloride,diphenyl methylene(fluorenyl)(3,5-dimethyl-2-phenoxy)titaniumdichloride, diphenylmethylene(fluorenyl)(3-tert-butyl-2-phenoxy)titanium dichloride,diphenyl methylene(fluorenyl)(3-tert-butyl-5-methyl-2-phenoxy)titaniumdichloride, diphenyl methylene(fluorenyl)(3-phenyl-2-phenoxy)titaniumdichloride, diphenyl methylene(fluorenyl)(3-tert-butyl dimethylsilyl-5-methyl-2-phenoxy)titanium dichloride, diphenylmethylene(fluorenyl)(3-trimethyl silyl-5-methyl-2-phenoxy)titaniumdichloride, diphenylmethylene(fluorenyl)(3-tert-butyl-5-methoxy-2-phenoxy)titaniumdichloride, diphenylmethylene(fluorenyl)(3-tert-butyl-5-chloro-2-phenoxy)titaniumdichloride, etc. and compounds in which titanium in these compounds ischanged into zirconium or hafnium, compounds in which dichloride ischanged into dibromide, diiodide, bis(dimethyl amide), bis(diethylamide), di-n-butoxide, or diiso propoxide, compounds in which(cyclopentadienyl), is changed into (dimethyl cyclopentadienyl),(trimethyl cyclopentadienyl), (n-butyl cyclopentadienyl), (tert-butyldimethyl silyl cyclopentadienyl), or (indenyl), transition metal complexwhose J in general formula [I] represents carbon atom, such as compoundsin which (3,5-dimethyl-2 phenoxy) is changed into (2 phenoxy),(3-methyl-2 phenoxy), (3,5-di-tert-butyl-2 phenoxy),(3-phenyl-5-methyl-2 phenoxy), (3-tert-butyl dimethyl silyl-2 phenoxy),or (3-trimethyl silyl-2 phenoxy), as well as dimethylsilyl(cyclopentadienyl)(2-phenoxies)titanium dichloride, dimethylsilyl(cyclopentadienyl)(3-methyl-2-phenoxy)titanium dichloride, dimethylsilyl(cyclopentadienyl)(3,5-dimethyl-2-phenoxy)titanium dichloride,dimethyl silyl(cyclopentadienyl)(3-tert-butyl-2-phenoxy)titaniumdichloride, dimethylsilyl(cyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titaniumdichloride, dimethyl silyl(cyclopentadienyl)(3,5-di-tert-butyl-2phenoxy)titanium dichloride, dimethylsilyl(cyclopentadienyl)(5-methyl-3-phenyl-2-phenoxy)titanium dichloride,dimethyl silyl(cyclopentadienyl)(3-tert-butyl dimethylsilyl-5-methyl-2-phenoxy)titanium dichloride, dimethylsilyl(cyclopentadienyl)(5-methyl-3-trimethyl silyl-2-phenoxy)titaniumdichloride, dimethylsilyl(cyclopentadienyl)(3-tert-butyl-5-methoxy-2-phenoxy)titaniumdichloride, dimethylsilyl(cyclopentadienyl)(3-tert-butyl-5-chloro-2-phenoxy)titaniumdichloride), dimethylsilyl(cyclopentadienyl)(3,5-diamyl-2-phenoxy)titanium dichloride,dimethyl silyl(methyl cyclopentadienyl)(2-phenoxies)titanium dichloride,dimethyl silyl(methyl cyclopentadienyl)(3-methyl-2-phenoxy)titaniumdichloride, dimethyl silyl(methylcyclopentadienyl)(3,5-dimethyl-2-phenoxy)titanium dichloride, dimethylsilyl(methyl cyclopentadienyl)(3-tert-butyl-2-phenoxy)titaniumdichloride, dimethyl silyl(methylcyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium dichloride,dimethyl silyl(methylcyclopentadienyl)(3,5-di-tert-butyl-2-phenoxy)titanium dichloride,dimethyl silyl(methylcyclopentadienyl)(5-methyl-3-phenyl-2-phenoxy)titanium dichloride,dimethyl silyl(methyl cyclopentadienyl)(3-tert-butyl dimethylsilyl-5-methyl-2-phenoxy)titanium dichloride, dimethyl silyl(methylcyclopentadienyl)(5-methyl-3-trimethyl silyl-2-phenoxy)titaniumdichloride, dimethyl silyl(methylcyclopentadienyl)(3-tert-butyl-5-methoxy-2-phenoxy)titanium dichloride,dimethyl silyl(methylcyclopentadienyl)(3-tert-butyl-5-chloro-2-phenoxy)titanium dichloride,dimethyl silyl(methyl cyclopentadienyl)(3,5-diamyl-2-phenoxy)titaniumdichloride, dimethyl silyl(n-butylcyclopentadienyl)(2-phenoxies)titanium dichloride, dimethylsilyl(n-butyl cyclopentadienyl)(3-methyl-2-phenoxy)titanium dichloride,dimethyl silyl(n-butyl cyclopentadienyl)(3,5-dimethyl-2-phenoxy)titaniumdichloride, dimethyl silyl(n-butylcyclopentadienyl)(3-tert-butyl-2-phenoxy)titanium dichloride, dimethylsilyl(n-butyl cyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titaniumdichloride, dimethyl silyl(n-butylcyclopentadienyl)(3,5-di-tert-butyl-2-phenoxy)titanium dichloride,dimethyl silyl(n-butylcyclopentadienyl)(5-methyl-3-phenyl-2-phenoxy)titanium dichloride,dimethyl silyl(n-butyl cyclopentadienyl)(3-tert-butyl dimethylsilyl-5-methyl-2-phenoxy)titanium dichloride, dimethyl silyl(n-butylcyclopentadienyl)(5-methyl-3-trimethyl silyl-2-phenoxy)titaniumdichloride, dimethyl silyl(n-butylcyclopentadienyl)(3-tert-butyl-5-methoxy-2-phenoxy)titanium dichloride,dimethyl silyl(n-butylcyclopentadienyl)(3-tert-butyl-5-chloro-2-phenoxy)titanium dichloride,dimethyl silyl(n-butyl cyclopentadienyl)(3,5-diamyl-2-phenoxy)titaniumdichloride, dimethyl silyl(tert-butylcyclopentadienyl)(2-phenoxy)titanium dichloride, dimethylsilyl(tert-butyl cyclopentadienyl)(3-methyl-2-phenoxy)titaniumdichloride, dimethyl silyl(tert-butylcyclopentadienyl)(3,5-dimethyl-2-phenoxy)titanium dichloride, dimethylsilyl(tert-butyl cyclopentadienyl)(3-tert-butyl-2-phenoxy)titaniumdichloride, dimethyl silyl(tert-butylcyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium dichloride,dimethyl silyl(tert-butylcyclopentadienyl)(3,5-di-tert-butyl-2-phenoxy)titanium dichloride,dimethyl silyl(tert-butylcyclopentadienyl)(5-methyl-3-phenyl-2-phenoxy)titanium dichloride,dimethyl silyl(tert-butyl cyclopentadienyl)(3-tert-butyl dimethylsilyl-5-methyl-2-phenoxy)titanium dichloride, dimethyl silyl(tert-butylcyclopentadienyl)(5-methyl-3-trimethyl silyl-2-phenoxy)titaniumdichloride, dimethyl silyl(tert-butylcyclopentadienyl)(3-tert-42-butyl-5-methoxy-2-phenoxy)titaniumdichloride, dimethyl silyl(tert-butylcyclopentadienyl)(3-tert-butyl-5-chloro-2-phenoxy)titanium dichloride,dimethyl silyl(tert-butylcyclopentadienyl)(3,5-diamyl-2-phenoxy)-titanium dichloride, dimethylsilyl(tetramethyl, cyclopentadienyl)(2-phenoxy)titanium dichloride,dimethyl silyl(tetramethylcyclopentadienyl)(3-methyl-2-phenoxy)-titanium dichloride, dimethylsilyl(tetramethyl cyclopentadienyl)(3,5-dimethyl-2-phenoxy)titaniumdichloride, dimethyl silyl(tetramethylcyclopentadienyl)(3-tert-butyl-2-phenoxy)titanium dichloride, dimethylsilyl(tetramethylcyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium dichloride,dimethyl silyl(tetramethylcyclopentadienyl)(3,5-di-tert-butyl-2-phenoxy)titanium dichloride,dimethyl silyl(tetramethylcyclopentadienyl)(5-methyl-3-phenyl-2-phenoxy)titanium dichloride,dimethyl silyl(tetramethyl cyclopentadienyl)(3-tert-butyl dimethylsilyl-5-methyl-2-phenoxy)titanium dichloride, dimethyl silyl(tetramethyl cyclopentadienyl)(5-methyl-3-trimethylsilyl-2-phenoxy)titanium dichloride, dimethyl silyl(tetramethylcyclopentadienyl)(3-tert-butyl-5-methoxy-2-phenoxy)titanium dichloride,dimethyl silyl(tetramethylcyclopentadienyl)(3-tert-butyl-5-chloro-2-phenoxy)titanium dichloride,dimethyl silyl(tetramethylcyclopentadienyl)(3,5-diamyl-2-phenoxy)titanium dichloride, dimethylsilyl(trimethyl silyl cyclopentadienyl)(2 phenoxy)titanium dichloride,dimethyl silyl(trimethyl silylcyclopentadienyl)(3-methyl-2-phenoxy)titanium dichloride, dimethylsilyl(trimethyl silyl cyclopentadienyl)(3,5-dimethyl-2-phenoxy)titaniumdichloride, dimethyl silyl(trimethyl silylcyclopentadienyl)(3-tert-butyl-2-phenoxy)titanium dichloride, dimethylsilyl(trimethyl silylcyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium dichloride,dimethyl silyl(trimethyl silylcyclopentadienyl)(3,5-di-tert-butyl-2-phenoxy)titanium dichloride,dimethyl silyl(trimethyl silylcyclopentadienyl)(5-methyl-3-phenyl-2-phenoxy)titanium dichloride),dimethyl silyl(trimethyl silyl cyclopentadienyl)(3-tert-butyl dimethylsilyl-5-methyl-2-phenoxy)titanium dichloride, dimethyl silyl(trimethylsilyl cyclopentadienyl)(5-methyl-3-trimethyl silyl-2-phenoxy)titaniumdichloride, dimethyl silyl(trimethyl silylcyclopentadienyl)(3-tert-butyl-5-methoxy-2-phenoxy)titanium dichloride,dimethyl silyl(trimethyl silylcyclopentadienyl)(3-tert-butyl-5-chloro-2-phenoxy)titanium dichloride,dimethyl silyl(trimethyl silylcyclopentadienyl)(3,5-diamyl-2-phenoxy)titanium dichloride, dimethylsilyl(indenyl)(2-phenoxy)titanium dichloride, dimethylsilyl(indenyl)(3-methyl-2-phenoxy)titanium dichloride, dimethylsilyl(indenyl)(3,5-dimethyl-2-phenoxy)titanium dichloride, dimethylsilyl(indenyl)(3-tert-butyl-2-phenoxy)titanium dichloride, dimethylsilyl(indenyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium dichloride,dimethyl silyl(indenyl)(3,5-di-tert-butyl-2-phenoxy)titanium dichloride,dimethyl silyl(indenyl)(5-methyl-3-phenyl-2-phenoxy)titanium dichloride,dimethyl silyl(indenyl)(3-tert-butyl dimethylsilyl-5-methyl-2-phenoxy)titanium dichloride, dimethylsilyl(indenyl)(5-methyl-3-trimethyl silyl-2-phenoxy)titanium dichloride,dimethyl silyl(indenyl)(3-tert-butyl-5-methoxy-2-phenoxy)titaniumdichloride, dimethylsilyl(indenyl)(3-tert-butyl-5-chloro-2-phenoxy)titanium dichloride,dimethyl silyl(indenyl)(3,5-diamyl-2-phenoxy)titanium dichloride,dimethyl silyl(fluorenyl)(2-phenoxy)titanium dichloride, dimethylsilyl(fluorenyl)(3-methyl-2-phenoxy)titanium dichloride, dimethylsilyl(fluorenyl)(3,5-dimethyl-2-phenoxy)titanium dichloride, dimethylsilyl(fluorenyl)(3-tert-butyl-2-phenoxy)titanium dichloride, dimethylsilyl(fluorenyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium dichloride,dimethyl silyl(fluorenyl)(3,5-di-tert-butyl-2-phenoxy)titaniumdichloride, dimethylsilyl(fluorenyl)(5-methyl-3-phenyl-2-phenoxy)titanium dichloride,dimethyl silyl(fluorenyl)(3-tert-butyl dimethylsilyl-5-methyl-2-phenoxy)titanium dichloride, dimethylsilyl(fluorenyl)(5-methyl-3-trimethyl silyl-2-phenoxy)titaniumdichloride, dimethylsilyl(fluorenyl)(3-tert-butyl-5-methoxy-2-phenoxy)titanium dichloride,dimethyl silyl(fluorenyl)(3-tert-butyl-5-chloro-2-phenoxy)titaniumdichloride, dimethyl silyl(fluorenyl)(3,5-diamyl-2-phenoxy)titaniumdichloride, dimethyl silyl(tetramethylcyclopentadienyl)(1-naphthoxy-2-yl)titanium dichloride etc., andtransition metal complexes whose J in general formula [1] representsatom of the 14th group of periodic table of elements other than carbonatom, such as, compounds in which in these compounds (cyclopentadienyl)is changed into (dimethyl cyclopentadienyl), (trimethylcyclopentadienyl), (ethyl cyclopentadienyl), (n-propylcyclopentadienyl), (isopropyl cyclopentadienyl), (sec-butylcyclopentadienyl), (isobutyl cyclopentadienyl), (tert-butyl dimethylsilyl cyclopentadienyl), (phenyl cyclopentadienyl), (methyl indenyl), or(phenyl indenyl), in which (2-phenoxy) is changed into(3-phenyl-2-phenoxy), (3-trimethyl silyl-2-phenoxy), or (3-tert-butyldimethyl silyl-2-phenoxy), in which dimethyl silyl is changed intodiethyl silyl, diphenyl silyl, or dimethoxy silyl, in which titanium ischanged into zirconium or hafnium, compounds in which dichloride ischanged into dibromide, diiodide, bis(dimethyl amide), bis(diethylamide), di-n-butoxide, or di-isopropoxide may be mentioned.

As transition metal complexes represented by general formula [II], forexample, μ-oxo-bis{isopropylidene(cyclopentadienyl)(2-phenoxy)titaniumchloride}, μ-oxo-bis{isopropylidene(cyclopentadienyl)(2-phenoxy)titaniummethoxide},μ-oxo-bis{isopropylidene(cyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titaniumchloride},μ-oxo-bis{isopropylidene(cyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titaniummethoxide}, μ-oxo-bis{isopropylidene(methylcyclopentadienyl)(2-phenoxy)titanium chloride},μ-oxo-bis{isopropylidene(methyl cyclopentadienyl)(2-phenoxy)titaniummethoxide}, μ-oxo-bis{isopropylidene(methylcyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium chloride},μ-oxo-bis{isopropylidene(methylcyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium methoxide},μ-oxo-bis{isopropylidene(tetramethyl cyclopentadienyl)(2phenoxies)titanium chloride}, μ-oxo-bis{isopropylidene(tetramethylcyclopentadienyl)(2-phenoxy)titanium methoxide},μ-oxo-bis{isopropylidene(tetramethylcyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium chloride},μ-oxo-bis{isopropylidene(tetramethylcyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium methoxide},μ-oxo-bis{dimethyl silylene(cyclopentadienyl)(2-phenoxy)titaniumchloride}, μ-oxo-bis{dimethylsilylene(cyclopentadienyl)(2-phenoxy)titanium methoxide},μ-oxo-bis{dimethylsilylene(cyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titaniumchloride}, μ-oxo-bis{dimethylsilylene(cyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titaniummethoxide}, μ-oxo-bis{dimethyl silylene(methylcyclopentadienyl)(2-phenoxy)titanium chloride}, μ-oxo-bis{dimethylsilylene(methyl cyclopentadienyl)(2-phenoxy)titanium methoxide},μ-oxo-bis{dimethyl silylene(methylcyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium chloride},μ-oxo-bis{dimethyl silylene(methylcyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium methoxide},μ-oxo-bis{dimethyl silylene(tetramethylcyclopentadienyl)(2-phenoxy)titanium chloride}, μ-oxo-bis{dimethylsilylene(tetramethyl cyclopentadienyl)(2-phenoxy)titanium methoxide},μ-oxo-bis{dimethyl silylene(tetramethylcyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium chloride},μ-oxo-bis{dimethyl silylene(tetramethylcyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium methoxide)etc. may be mentioned.

As transition metal complex represented by general formula [III], forexample,di-μ-oxo-bis{isopropylidene(cyclopentadienyl)(2-phenoxy)titanium},di-μ-oxo-bis{isopropylidene(cyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium},di-μ-oxo-bis{isopropylidene(methylcyclopentadienyl)(2-phenoxy)titanium},di-μ-oxo-bis{isopropylidene(methylcyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium},di-oxo-bis{isopropylidene(tetramethyl cyclopentadienyl)(2-phenoxytitanium}, di-mu-oxo-bis{isopropylidene(tetramethylcyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium},di-mu-oxo-bis{dimethyl silylene(cyclopentadienyl)(2-phenoxy)titanium},di-μ-oxo-bis{dimethylsilylene(cyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium},di-μ-oxo-bis{dimethyl silylene(methylcyclopentadienyl)(2-phenoxy)titanium}, di-μ-oxo-bis{dimethylsilylene(methylcyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium},di-μ-oxo-bis{dimethyl silylene(tetramethylcyclopentadienyl)(2-phenoxy)titanium}, di-μ-oxo-bis{dimethylsilylene(tetramethylcyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium} etc. may bementioned.

Transition metal complexes represented by the above-mentioned generalformula [I], for example, may be manufactured by a method described inWO097/03992 laid open specification. Moreover, transition metal complexrepresented by the above-mentioned general formula [II] or [III] may bemanufactured by reacting transition metal complex represented by theabove-mentioned general formula [I] with one chemical equivalent or twochemical equivalents of water.

(β) Description about aluminum compounds will be given in thisparagraph.

As aluminum compounds (β), one or more kinds of aluminum compoundschosen from following (β1)-(β3) are mentioned.

-   -   (β1) Organic aluminum compounds represented by a general formula        E¹ ₃aAlZ_(3-a)    -   (β2) Cyclic aluminoxanes that has a structure represented by a        general formula {—Al(E²)—O—}_(b)    -   (β3) Linear aluminoxanes that has a structure represented by a        general formula E³{—Al(E³)—O—}_(c)AlE³ ₂    -   (where E¹, E², and E³ represent hydrocarbon groups,        respectively, and all E¹, all E², and all E³ may be the same, or        they may be different from each other. Z represents hydrogen        atom or halogen atom, and all Z may be the same, or may be        different from each other. Character are presents a number that        satisfies 0<a ≦3, b an integer of two or more, and c an integer        of one or more.)

As hydrocarbon groups in E¹, E², or E³, hydrocarbon groups with 1-8carbons are preferable, and alkyl groups are more preferable.

As examples of organic aluminum compounds (β1) represented by a generalformula E¹ _(a)AlZ_(3-a); trialkyl aluminums, such as trimethylaluminum, triethyl aluminum, tripropyl aluminum, triisobutyl aluminum,and trihexyl aluminum; dialkyl aluminum chlorides, such as dimethylaluminum chloride, diethyl aluminum chloride, dipropyl aluminumchloride, diisobutyl aluminum chloride, and dihexyl aluminum chloride;alkyl aluminum dichlorides, such as methyl aluminum dichloride, ethylaluminum dichloride, propyl aluminum dichloride, isobutyl aluminumdichloride, and hexyl aluminum dichloride; dialkyl aluminum hydrides,such as dimethyl aluminum hydride, diethyl aluminum hydride, dipropylaluminum hydride, diisobutyl aluminum hydride, and dihexyl aluminumhydride, etc. may be mentioned. Preferably, trialkyl aluminum may bementioned and more preferably triethyl aluminum or triisobutyl aluminum.

As examples of E² and E³ in a cyclic aluminoxane (β2) that has astructure represented by a general formula {—Al(E²)—O—}_(b), and linearan aluminoxanes (β3) that have a structure represented by a generalformula E³{—Al(E³)—O—}_(c)AlE³ ₂, alkyl groups, such as methyl group,ethyl group, normal propyl group, isopropyl group, normal butyl group,isobutyl group, normal pentyl group, and neopentyl group may bementioned. Character b represents an integer of two or more, and crepresents an integer of one or more. Preferably, E² and E³ representmethyl group or isobutyl group, and b represents 2-40 and c represents1-40.

The above-mentioned aluminoxanes may be made by various kinds ofmethods. Methods of manufacturing the aluminoxanes do not have anylimitation, and they may be manufactured according to well-knownmethods. For example, an alminoxane is obtained by contacting a solutionin which a trialkyl aluminum (for example, trimethyl aluminum etc.) isdissolved in suitable organic solvents (benzene, aliphatic hydrocarbon,etc.) with water. Moreover, a method of contacting a trialkyl aluminum(for example, trimethyl aluminum etc.) with metal salts (for example,copper sulfate hydrate etc.) containing water of crystallization may bementioned.

(γ) Description about boron compounds will be given in this paragraph.

As boron compounds (γ), any one selected from (γ1) boron compoundsrepresented by a general formula BQ¹Q²Q³, and (γ2) boron compoundsrepresented by a general formula G⁺(BQ¹Q²Q³Q⁴)⁻, and (γ3) boroncompounds represented by a general formula (L-H)⁺(BQ¹Q²Q³Q⁴)⁻ may beused.

In boron compounds (β1) represented by a general formula BQ¹Q²Q³, Brepresents boron atom of trivalent valence state, Q¹ to Q³ representhalogen atom, hydrocarbon group, halogenated hydrocarbon group,substituted silyl group, alkoxy group, or di-substituted amino group,and they may be the same, or different from each other. As Q¹ to Q³halogen atom, hydrocarbon group containing 1-20 carbon atoms,halogenated hydrocarbon group containing 1-20 carbon atoms, substitutedsilyl group containing 1-20 carbon atoms, alkoxy group containing 1-20carbon atoms, or amino group containing 2-20 carbon atoms may bepreferably mentioned, and more preferably Q¹ to Q³represent halogenatom, hydrocarbon group containing 1-20 carbon atoms, or halogenatedhydrocarbon containing 1-20 carbon atoms. Still more preferably, Q¹ toQ⁴ represent fluorinated hydrocarbon group with 1-20 carbon atomscontaining at least one fluorine atom, respectively, and furthermorepreferably Q¹ to Q⁴ represent fluorinated aryl group with 6-20 carbonatoms containing at least one fluorine atom, respectively.

As an example of compounds (γ1), tris(pentafluoro phenyl)boran,tris(2,3,5,6-tetrafluoro phenyl)boran, tris(2,3,4,5-tetrafluorophenyl)boran, tris(3,4,5-trifluoro phenyl)boran, tris(2,3,4-trifluorophenyl)boran, phenyl bis(penta fluoro phenyl boran, etc. may bementioned, and most preferably tris(pentafluoro phenyl)boran may bementioned.

In boron compounds (γ2) represented by a general formula G⁺(BQ¹Q²Q³Q⁴),G⁺ represents a, inorganic or organic cation, and B represents boronatom of trivalent valence state, and Q¹ to Q⁴ are the same as Q¹ to Q³in above (γ1).

As example of G⁺ that represents an inorganic cation in compoundsrepresented by a general formula G⁺(BQ¹Q²Q³Q⁴)⁻, ferrocenium cation,alkyl substituted ferrocenium cation, silver cation, etc. may bementioned, and triphenylmethyl cation etc. may be mentioned as G⁺ thatrepresents organic cation. As G⁺, carbenium cation may be preferablymentioned, and especially preferably triphenylmethyl cation. As(BQ¹Q²Q³Q⁴)⁻, tetrakis(penta fluoro phenyl borate,tetrakis(2,3,5,6-tetrafluoro phenyl)borate, tetrakis(2,3,4,5-tetrafluorophenyl)borate, tetrakis(3,4,5-trifluoro phenyl)borate,tetrakis(2,3,4-trifluoro phenyl)borate, phenyltris(penta fluorophenyl)borate, tetrakis(3,5-bistrifluoro methyl phenyl)borate, etc. maybe mentioned.

As practical examples of these compounds, ferroceniumtetrakis(pentafluorophenyl)borate, 1,1-dimethylferroceniumtetrakis(pentafluoro phenyl)borate, silver tetrakis(pentafluorophenyl)borate, triphenylmethyl tetrakis(penta fluoro phenyl)borate,triphenylmethyl tetrakis (3,5-bistrifluoro methyl phenyl)borate, etc.may be mentioned, and most preferably triphenylmethyltetrakis(pentafluoro phenyl)borate may be mentioned.

Moreover, in boron compounds (γ3) represented by a general formula(L-H)⁺(BQ¹Q²Q³Q⁴)⁻, L represents neutral Lewis bases, (L-H)⁺ representsBroensted acids, B represents boron atom of trivalent valence state, andQ¹ to Q⁴ are the same as Q¹ to Q³ in the above-mentioned Lewis acid(γ1).

As an example of (L-H)⁺ that represents Broensted acid in compoundrepresented with general formula (L-H)⁺(BQ¹Q²Q³Q⁴)⁻, trialkylsubstituted ammonium, N, and N-dialkyl anilinium, dialkyl ammonium,triaryl phosphonium, etc. are mentioned, and as (BQ¹Q²Q³Q⁴)⁻, the sameexample as the above-mentioned description may be mentioned.

As practical examples of these compounds, triethyl ammoniumtetrakis(pentafluoro phenyl)borate, tripropyl ammoniumtetrakis(pentafluoro phenyl)borate, tri(n-butyl)ammoniumtetrakis(pentafluoro phenyl)borate, tri(n-butyl)ammoniumtetrakis(3,5-bistrifluoromethyl phenyl)borate, N,N-dimethylaniliniumtetrakis(pentafluoro phenyl)borate, N,N-diethyl aniliniumtetrakis(pentafluoro phenyl)borate, N,N-2,4,6-pentamethyl aniliniumtetrakis(pentafluoro phenyl)borate, N,N-dimethyl aniliniumtetrakis(3,5-bistrifluoromethyl phenyl)borate, diisopropyl ammoniumtetrakis(pentafluoro phenyl)borate, dicyclohexylammoniumtetrakis(pentafluoro phenyl)borate, triphenyl phosphoniumtetrakis(pentafluoro phenyl)borate, tri(methyl phenyl)phosphoniumtetrakis(pentafluoro phenyl)borate, tri(dimethyl phenyl)phosphoniumtetrakis(pentafluoro phenyl)borate, etc. may be mentioned, and mostpreferably tri(n-butyl)ammonium tetrakis(pentafluoro phenyl)borate orN,N-dimethyl anilinium tetrakis(pentafluoro phenyl)borate may bementioned.

In copolymerization, a transition metal complex (α), and a catalyst forolefin polymerization in which the above-mentioned (β) and/or theabove-mentioned (γ) are used. When a catalyst for olefin polymerizationthat consists of two component of (α) and (β) is used, as (β), theabove-mentioned cyclic aluminoxane (β2) and/or the above-mentionedlinear aluminoxane (β3) are preferable. Moreover, as another preferableembodiment of a catalyst for olefin polymerization, the above-mentionedcatalyst for olefin polymerization in which the above-mentioned (α),(β), and (γ) are used may be mentioned, and as the (β), theabove-mentioned (β) is easily used in the case.

Usually, each component is preferably used in an amount of mole ratio ina range that (β)/(α) is 0.1-10000, preferably 5-2000, and mole ratio ina range that (γ)/(α) is 0.01-100, preferably 0.5-10.

Concentration is suitably chosen based on conditions, such asperformance of equipment that supplies each component to apolymerization reactor, in the case where each component is used in asolution state or in a state of suspension in solvent. Generally eachcomponent is used so that (α) is usually in a range of 0.01-500 μmol/g,more preferably 0.05-100 μmol/g, and still preferably, 0.05-50 μmol/g.And generally each component is used so that (β) is usually in a rangeof 0.01-10000 μmol/g, as Al atom converted value, more preferably0.1-5000 μmol/g, and still preferably 0.1-2000 μmol/g. Moreover, eachcomponent is used so that (γ) is usually in a range of 0.01-500 μmol/g,more preferably 0.05-200 μmol/g, and still preferably, 0.05-100 μmol/g.

In order to manufacture olefin derived copolymers, a solventpolymerization method or a slurry polymerization method in whichaliphatic hydrocarbons, such as butane, pentane, hexane, heptane, andoctane, aromatic hydrocarbons, such as benzene and toluene, orhalogenated hydrocarbons, such as methylene dichloride, are used as asolvent, and a vapor phase polymerization method in gas-phase monomer,etc. may be used. Moreover, either continuous polymerization method orbatch cycle polymerization method may be used. A polymerizationtemperature may be adopted the range of −50 to 200 degrees C., and arange of −20 to 100 degrees C. is especially preferable. As forpolymerization pressure, atmospheric pressure to 60 kg/cm²G ispreferable. Generally polymerization time may be decided suitably basedon a kind of catalyst used, and reaction equipments, and the range ofone minute-20 hours may be adopted. Moreover, in order to adjust amolecular weight of polymer, a chain-transferring agent, such ashydrogen, may also be added.

Subsequently, thermoplastic resin compositions in the present inventionobtained from new olefin derived copolymers and thermoplastic resinswill be described.

Thermoplastic resin compositions of the present invention arethermoplastic resin compositions that consist of 1-99 weight % of (i)thermoplastic resins, and 99-1 weight % of (ii) olefin derivedcopolymers of the present invention.

Preferably, thermoplastic resin compositions of the present inventionare thermoplastic resin compositions that consist of 5-95 weight % of(i) thermoplastic resins and, 95-5 weight % of (ii) olefin derivedcopolymers of the present invention, more preferably thermoplastic resincompositions that consist of 10-90 weight % of (i) thermoplastic resins,and 90-10 weight % of (ii) olefin derived copolymers of the presentinvention, still more preferably thermoplastic resin compositions thatconsist of 15-85 weight % of (i) thermoplastic resins and, and 85-15% of(ii) olefin derived copolymers of the present invention, and especiallypreferably thermoplastic resin compositions that consist of 20-80 weight% of (i) thermoplastic resins and, 80-20 weight % of (ii) olefin derivedcopolymers of the present invention.

Components (i) used for thermoplastic resin compositions of the presentinvention are thermoplastic resins. (i) may be widely selected fromvarious well-known thermoplastic resins, for example, polyethylenederived resins, such as high-density polyethylene and middle-densitypolyethylene, low-density polyethylene,-and linear low-densitypolyethylene (LLDPE); polypropylene derived resins; polybutene derivedresins: poly-4-methyl-pentene-1 derived resins; polystyrene derivedresins; polyester derived resins; polyamide derived resins; polyphenyleneether derived resins; polyphenylene oxide-resins; polyacetalderived resins; polycarbonate derived resins, etc. may be mentioned.Preferably, (i) are (i-1) polyolefin derived resins, more preferablypolyolefin derived resins that have (i-2) aliphatic olefins with two ormore carbons, as main components, more preferably, (i-3) poly olefinderived resins that have aliphatic olefins with three or more carbons asmain components, and especially preferably (i-4) polypropylene derivedresins.

As (i-4) polypropylene derived resins, crystalline polypropylenes thatmainly have isotactic or syndiotactic sequence structure. Polypropylenesof such as homogeneous type, random type containing comonomer, or blocktype by multi-stage polymerization that have structures in a wide rangemay be used. In addition, as a polymerization method of thepolypropylene derived resins, a vapor phase polymerization method, abulk polymerization method, a solvent polymerization method, and amulti-stage polymerization in which the above-mentioned methods arecombined arbitrarily are employable. Moreover, there is especially nolimitation in a number average molecular weight of polymer, and it ispreferably adjusted to 10000-1000000.

As indexes of crystalline state of (i-4) polypropylene derived resins,for example, a melting point, an amount of crystal melting calorie, etc.are used. A melting point is preferably in a range of 80 degrees C.-176degrees C., and, an amount of crystal melting calorie is preferably isin a range of 30 J/g-120 J/g. More preferably, a melting point is in arange of 120 degrees C.-176 degrees C., and an amount of crystal meltingcalorie in a range of 60 J/g-120 J/g. If a melting point is too low oran amount of heat of fusion is too small, heat resistance ofthermoplastic resin compositions and a molded body containingthermoplastic resin compositions obtained may be decreased.

Following methods are used as methods of manufacturing (i-4)polypropylene derived resins. Generally as catalysts, so-calledZiegler-Natta type catalysts in which transition metal components in ashape of a solid containing titanium and organic metal components arecombined, or metallocene catalysts that consist of transition metalcompounds of the 4th group—the 6th group of periodic table with at leastone cyclopentadienyl frame and co-catalyst components are used. Aspolymerization methods, slurry polymerization, vapor phasepolymerization, bulk polymerization, solution polymerization, etc. areused, or methods in which the above-mentioned methods are combined areused in one-step or multi-step to obtain homopolymerized polypropylenes.Moreover, copolymerized polypropylenes may be obtained by copolymerizingpropylene with one or more olefins selected from olefins having 2-12carbons other than propylene in one-step or multi-step using theabove-mentioned methods. In addition, it is also possible to usecommercially available materials.

In thermoplastic resin compositions and a molded body containingthermoplastic resin compositions of the present invention, whenflexibility, transparency, resistance to whitening, scratch resistance,and excellent performance balance are required, it is preferable that(i) are polypropylene derived resins (i-6) in which 15 or more to 205 orless of methylene carbons in two or more chains are contained in 1000carbon chains as main chain. More preferably, 25 or more to 155 or lessof methylene carbons in two or more chains are contained in 1000 carbonchains as main chain, and still more preferably 35 or more to 105 orless. If (i-6) goes out of the range, flexibility, transparency,resistance to whitening, and scratch resistance of thermoplastic resincompositions and a molded body containing thermoplastic resincompositions obtained may be decreased. As methods of having apredetermined number of methylene carbons of two or more chainscontained into (i-6), a method of copolymerizing ethylene to propylene,and a method of forming tail-to-tail bonds of propylene may bementioned. Content of methylene carbons of two or more chains containedin 1000 carbon chains of (i-6) as main chain can be measured using¹³C-NMR, IR, etc. The analysis method of ¹³C-NMR and IR is indicated inNew Edition Macromolecule Analysis Handbook 1.2.3 (1995).

When performance excellent in shock resistance and resistance towhitening is required for a molded body containing thermoplastic resincompositions and thermoplastic resin compositions of the presentinvention, it is preferable that (i) are polypropylene derived resincompositions (i-7) obtained by having ethylene and propylenecopolymerized in two or more steps. In detail, (i-7) represents thefollowing compositions: in a first step, a photopolymer of propylene, orethylene propylene copolymer having 5.0 or less weight % of ethylenecontent is obtained, and in a second step or after, ethylene propylenecopolymer having 7-85 weight % of ethylene content is obtained, and atthe same time, a weight ratio of a polymer obtained in a first step to apolymer obtained in a second step or after is 30/70-90/10. (A propylenehomopolymer or ethylene propylene copolymer obtained in a polymerizationof a first step may be denoted as “copolymer-1” hereinafter. Andethylene propylene copolymer obtained in a copolymerization in a secondstep or after may be denoted as “copolymer-2”.)

Ethylene content of the copolymer-1 is preferably 5.0 or less weight %.If ethylene content exceeds 5.0 weight %, heat resistance ofthermoplastic resin compositions and a molded body containingthermoplastic resin compositions obtained using the polypropylenederived resin compositions may be decreased.

Eethylene content of the copolymer-2 is preferably 7-85 weight %. Theresistance to whitening of thermoplastic resin compositions obtainedusing the polypropylene derived resin compositions may be decreased whenethylene content is too small. Alternatively when ethylene content isexcessive, shock resistance of thermoplastic resin compositions and amolded body containing thermoplastic resin compositions obtained usingthe polypropylene derived resin compositions may be decreased.

A weight ratio of the copolymer-1 and the copolymer-2 is 30/70-90/10.When a content of the copolymer-1 is too little (the copolymer-2 isexcessive), thermoplastic resin compositions and, and a molded bodycontaining thermoplastic resin compositions obtained using thepolypropylene derived resin compositions cannot obtain sufficientresistance to whitening. On the other hand, when the copolymer-1 isexcessive (content of the copolymer-2 is too little), inadequate shockresistance may be obtained in the thermoplastic resin compositions andthe molded body containing thermoplastic resin compositions that areobtained using the polypropylene derived resin compositions.

In addition small quantity, for example, about one to five weight %, ofα-olefins other than propylene and ethylene (for example, butene-1,hexene-1, octene-1, etc.) may be contained in the copolymer-1 andcopolymer-2.

Common name of the above-mentioned polypropylene derived resins issometimes “block polypropylene” or “high impact polypropylene”, andcommercially available materials may be used.

When performance excellent in transparency, elongation, flexibility, andworkability is required for thermoplastic resin compositions, and amolded body containing thermoplastic resin compositions of the presentinvention, it is preferable that (i) is propylene-ethylene copolymers(i-8) that have JIS A hardness of 70-97 measured based on JIS K6301, andhave modulus of elasticity in bending measured based on JIS K7203 of50-500 MPa.

JIS A hardness of (i-8) measured based on JIS K6301 is preferably 70-97,more preferably 75-97. When the hardness is too small, heat resistanceof thermoplastic resin compositions obtained and a molded bodycontaining thermoplastic resin compositions may be decreased. On theother hand, when the hardness is excessive, flexibility of thermoplasticresin compositions obtained and a molded body containing thermoplasticresin compositions may be decreased.

Modulus of elasticity in bending of (i-8) measured based on JIS K7203 ispreferably 50-500 MPa, and more preferably is 55-450 MPa. When themodulus of elasticity in bending is too small, heat resistance ofthermoplastic resin composition and a molded body containingthermoplastic resin compositions obtained may be decreased, and when themodulus of elasticity in bending is excessive, on the other hand,flexibility of thermoplastic resin compositions and a molded bodycontaining thermoplastic resin compositions obtained may be decreased.

As each monomer component that constitutes copolymer (i-8), componentsthat have 1-85 mol % of monomer unit based on ethylene, and 99-15 mol %of monomer unit based on propylene are preferable. The monomer maycontain α-olefins other than ethylene, propylene, for example, 1-butene,4-methyl-1-pentene, 1-hexene, 3-methyl-1-butene; or non-conjugated dienemonomers, such as 1,4-hexadiene, dicyclopentadiene,5-ethylidene-2-norbornene, 7-methyl-1,6-octadiene in a range of 5 mol %or less.

Moreover, (i-8) may be copolymers obtained by copolymerizing monomersother than the above-mentioned monomers that have functional groups. Asthe functional groups, hydroxyl group, carboxyl group, acid anhydridegroup, amino group, isocyanate group, epoxy group, ester group, etc. maybe mentioned. As such monomers, for example, (meth)acrylic acid hydroxyacrylate, (anhydrous)maleic acid, glycidyl (meth)acrylate, etc. may bementioned. Moreover, propylene-ethylene copolymers are modified and theabove-mentioned functional groups may be introduced.

As (i-8), random type or block type copolymers by multi-stagepolymerization maybe mentioned. As polymerization methods, vapor phasepolymerization method, bulk polymerization method, solventpolymerization method, and multi-stage polymerization method in whichthe above-mentioned polymerization methods are arbitrarily combined maybe employable. Moreover, there is especially no limitation for a numberaverage molecular weight of the polymer, and it is preferably adjustedto 10000-1000000.

In addition, corresponding commercial materials may be used aspropylene-ethylene copolymers (i-8).

In the case where thermoplastic resin compositions and a molded bodycontaining thermoplastic resin composition of the present invention isrequired excellent performance in elongation, flexibility, transparency,and workability, in addition to (i-8) and (ii), poly olefin derivedresins (i-9) that have flexural modulus measured based on JIS K7203 of550-1800 MPa may be further contained.

Flexural modulus of (i-9) measured based on JIS K7203 is 550-1800 MPa,and preferably is 600-1800 MPa. When the modulus of elasticity inbending is too small, heat resistance of thermoplastic resincompositions and a molded body containing thermoplastic resincompositions obtained may be decreased, and when the modulus ofelasticity in bending is excessive, on the other hand, flexibility ofthermoplastic resin compositions and a molded body containingthermoplastic resin compositions obtained maybe decreased. In case ofusing (i-9), an amount preferably satisfies that an weight ratio of(amount of sum of (i) and (i-8))/(amount of (i-9) is 30/70-99/1. A goodbalance of flexibility and strength of thermoplastic resin compositionsand a molded body containing thermoplastic resin compositions obtainedmay be achieved using (i-9) in this range.

When performance excellent in transparency and flexibility is requiredfor thermoplastic resin compositions and a molded body containingthermoplastic resin compositions of the present invention, it ispreferable that (i) is (i-10) poly butene derived resins. (i-10) ispolybutene homopolymer resins or polybutene copolymer resins synthesizedby well-known technology using Ziegler-Natta type catalysts ormetallocene derived catalysts. It is preferable that a melting point of(i-10) measured by a differential scanning calorimeter (DSC) is 30-130degrees C., more preferably 40-130 degrees C., and especially preferably50-130 degrees C. When the melting point is too low, heat resistance andstrength of thermoplastic resin compositions and a molded bodycontaining thermoplastic resin compositions obtained using thispolybutene may be decreased. As a differential scanning calorimeter,DSC220C by SEIKO Electronic Ind., Co. is used, for example, andmeasurement is performed at the rate of 10 degrees C./min in both oftemperature rising and temperature fall process.

(i-10) is obtained by copolymerizing 1-butene with ethylene or α-olefinswith 3-8 carbons. Propylene, 1-hexene, 1-octene, etc. are mentioned aspreferable α-olefins. A percentage of the α-olefins, an amount of 50 orless weight % is used, preferably 5-40 weight %, and especiallypreferably one-30 weight %. In addition, commercially availablematerials may be used as (i-10).

When performance excellent in transparency and flexibility is requiredfor thermoplastic resin compositions and a molded body containingthermoplastic resin compositions of the present invention and strengthand heat resistance is further required, in addition to polybutenederived resins (i-10) and (ii), polypropylene derived resins (i-4) mayfurther be contained, and it is preferable that 1-98 weight % of (i-10),1-98 weight % of (ii), and 1-98 weight % of (i-4) may be contained.Furthermore, it is more preferable that 5-90 weight % of (i-10), and5-90 weight % of (ii), and 5-90 weight % of (i-4) maybe contained. When(ii) is too little, flexibility and transparency of thermoplastic resincompositions and a molded body containing thermoplastic resincompositions obtained may be decreased. On the other hand, when (ii) isexcessive, heat resistance and strength of thermoplastic resincompositions and a molded body containing thermoplastic resincompositions obtained may be decreased. When (i-10) is too little,flexibility and transparency of thermoplastic resin compositions and amolded body containing thermoplastic resin compositions obtained may bedecreased. On the other hand, when (i-10) is excessive, strength andheat resistance of thermoplastic resin compositions and a molded bodycontaining thermoplastic resin compositions obtained may be decreased.When (i-4) is too little, heat resistance and strength of thermoplasticresin compositions and a molded body containing thermoplastic resincompositions obtained may be decreased. When polypropylene derived resin(i-4) is excessive, on the other hand, flexibility and transparency ofthermoplastic resin compositions and a molded body containingthermoplastic resin compositions obtained may be decreased.

When performance excellent in transparency and heat resistance isrequired for thermoplastic resin compositions and a molded bodycontaining thermoplastic resin compositions of the present invention,cyclic olefin derived resins (i-5) may be used as (i).

(i-5) is cyclic olefin homopolymer resins or cyclic olefin copolymerresins synthesized by well-known technology using Ziegler-Natta typecatalysts or metallocene derived catalysts. As cyclic olefins, forexample, norbornene, 5-methyl norbornene, 5-ethyl norbornene, 5-propylnorbornene, 5,6-dimethyl norbornene, 1-methyl norbornene, 7-methylnorbornene, 5,5,6-trimethyl norbornene, 5-phenyl norbornene, 5-benzylnorbornene, 5-ethylidene norbornene, 5-vinyl norbornene,1,4,5,8-dimethano-1,2,3,4,4a,5,8,8a-octahydro naphthalene,2-methyl-1,4,5 8-dimethano-1,2,3,4,4a,5,8,8a-octahydro naphthalene,2-ethyl-1,4,5,8-dimethano-1,2,3,4,4a,5,8,8a-octahydro naphthalene,2,3-dimethyl-1,4,5,8-dimethano-1,2,3,4,4a,5,8,8a-octahydro naphthalene,2-hexyl-1,4,5,8-dimethano-1,2,3,4,4a,5,8,8a-octahydro naphthalene,2-ethylidene-1,4,5,8-dimethano 1,2,3,4,4a,5,8,8a-octahydro naphthalene,2-fluoro-1,4,5,8-dimethano-1,2,3,4,4a,5,8 8a-octahydro naphthalene,1,5-dimethyl-1,4,5,8-dimethano-1,2,3,4,4a,5,8,8a-octahydro naphthalene,2-cyclohexyl-1,4,5,8-dimethano-1,2,3,4,4a,5,8,8a-octahydro naphthalene,2,3-dichloro-1,4,5,8-dimethano-1,2,3,4,4a,5,8,8a-octahydro naphthalene,2-isobutyl-1,4,5,8-dimethano-1,2,3,4,4a,5,8,8a-octahydro naphthalene,1,2-dihydro dicyclopentadiene, 5-chloro norbornene, 5,5-dichloronorbornene, 5-fluoro norbornene, 5,5,6-trifluoro-6-trifluoro methylnorbornene, 5-chloro methyl norbornene, 5-methoxy norbornene,5,6-dicarboxyl norbornene anhydrate, 5-dimethylamino norbornene,5-cyanonorbornene, cyclopentene, 3-methylcyclopentene.4-methylcyclopentene, 3,4-dimethylcyclopentene,3,5-dimethylcyclopentene, 3-chlorocyclopentene, cyclohexene, 3-methylcyclohexene, 4-methyl cyclohexene, 3,4-dimethyl cyclohexene, 3-chlorocyclohexene, cyclo heptene, etc. may be mentioned.

(i-5) is obtained by copolymerizing cyclic olefins with ethylene orα-olefins with 3-8 carbons, and as preferable α-olefins, propylene,1-butene, 1-hexene, 1-octene, etc. may be mentioned. As for percentageof these alpha-olefins, an amount of 50 or less weight % is used,preferably 0.5-40 weight %, and especially preferably 1-30 weight %.

Thermoplastic resin compositions of the present invention consists of1-99 weight % of (i), and 99-1 weight % of (ii), (where (i)+(ii)=100weight %), preferably, 5-90 weight % of (i), and 95-10 weight % of (ii),more preferably, 10-80 weight % of (i), and 90-20 weight % of (ii),still more preferably, 15-70 weight % of (i) and 85-30 weight % of (ii),and especially preferably, 20-60 weight % of (i) and 80-40 weight % of(ii). When (i) is too small ((ii) is excessive), flexibility may bedecreased. On the other hand, when (ii) is excessive ((i) is toolittle), strength may be decreased.

In thermoplastic resin compositions of the present invention, it ispreferable that haze measured based on JIS K7105 of 1 mm thick pressmolded sheet is 75% or less, preferably, 70% or less, more preferably,65% or less, still preferably, 60% or less, and especially preferably,55% or less. When haze goes out of this range, flexibility,transparency, resistance to whitening, and scratch resistance ofthermoplastic resin compositions and a molded body containingthermoplastic resin compositions may be decreased. In addition, this 1mm thick press molded sheet must be a press molded sheet moldedaccording to a forming method of test piece indicated by JIS examinationmethod of thermoplastic resins contained in thermoplastic resincompositions. For example, if a thermoplastic resin contained inthermoplastic resin composition is polypropylene derived resin, pressmolded sheet molded by JIS K6758 according to the method of publicationmust be used. Attention must be paid to appearance, such as mixing ofair bubbles and foreign matters, to the molded sheet, and a portion inwhich they exist must not be used for evaluation.

In thermoplastic resin compositions of the present invention, it ispreferable that haze measured based on JIS K7105 after 50 degree C. and100-hour heat run test of 1 mm thick press molded sheet is 90% or less.A temperature of heat run test is preferably 70 degrees C., morepreferably 80 degrees C., still more preferably 90 degrees C., andespecially preferably 110 degrees C. When the haze goes out of thisrange, a surf ace character stability of thermoplastic resincompositions and a molded body containing thermoplastic resincompositions may be decreased. In addition, as a 1 mm thick press moldedsheet, a sheet obtained by the above-mentioned press molding method mustbe used.

In thermoplastic resin compositions of the present invention, it ispreferable that a haze value difference (Δ haze) measured based on JISK7105 before and after 50 degree C. and 100 hour heat run test of 1 mmthick molded sheet is 40 or less, more preferably 35 or less, still morepreferably 30 or less, further more preferably 25 or less, and mostpreferably 20 or less. Moreover, a temperature of the heat run test ispreferably 70 degrees C., more preferably 80 degrees C., still morepreferably 90 degrees C., and especially preferably 110 degrees C. Whenout of this range, a surface character stability of thermoplastic resincompositions and a molded body containing thermoplastic resincompositions may get inferior. In addition, as a 1 mm thick press moldedsheet, a sheet obtained by the above-mentioned press molding method mustbe used. Moreover, the heat run test of 50 degree C. and 100 hours for 1mm thick molded sheet must be carried out based on air heating agingtest (6.3) of JIS K6301 “6. Aging test”, except that examinationtemperature is set at 50 degrees C., and examination time for 100 hours.By hanging and heating the test pieces in testing machine tub, at thistime, the test pieces hung must not contact mutually, and they must nottouch any portion of wall in the testing machine tub.

In thermoplastic resin compositions of the present invention, it ispreferable that modulus of elasticity in bending (Ub (MPa)) measuredbased on JIS K7203 satisfies a relationship of the following expression.

 Ub≦1.5×Sb×(Tb/100)^(3.3),more preferably Ub≦1.4×Sb×(Tb/100)^(3.3)still more preferably, Ub≦1.3×Sb×(Tb/100)^(3.3), andespecially preferably Ub≦1.2×Sb×(Tb/100)^(3.3).

When Ub goes out of the above-mentioned range, flexibility,transparency, resistance to whitening, and scratch resistance ofthermoplastic resin compositions and a molded body containingthermoplastic resin compositions may be decreased. In addition, in theabove-mentioned expression, Sb represents flexural modulus (MPa)measured based on JIS K7203of (a), and Tb represents an added weightpart (%) of (a) in thermoplastic resin compositions.

Furthermore, thermoplastic resin compositions of the present inventionis specialized in a gloss value change before and after examination of 1or less, when a molded sheet with 2 or less of surface gloss, and withembossed pattern obtained using the composition by molding according tothe below-mentioned conditions undergoes a heat run test of 110 degreeC. and 100 hours. When the gloss change value becomes equal to or morethan the range, decline in surface quality (stickiness etc.) ofthermoplastic resin compositions and a molded body containingthermoplastic resin compositions may be induced. In addition, heat runtest of 110 degree C. and 100 hours of molded sheet with embossedpattern having two or less surface gloss is carried out by the followingmethod. Press molded sheet of 1 mm thick (15 cm square) with Glen Cgranulated leather embossed pattern is prepared using press moldingmachine so that the surface gloss value with granulated leather embossedpattern measured by the following method may be two or less. Inaddition, a press molding is performed using the same type of moldingmachine under the conditions of pressurized cooling method (50 kg/cm²G,upper and lower plate with water cooling), after raw material is heatedand melted for 5 minutes under conditions of upper and lower plate at200 degrees C., 5 kg/cm² G. This sheet is cut into a rectanglar by 5cm×3 cm, and subsequently is laid so that the surface with granulatedleather embossed pattern may be upper surface in Gear oven aging tester(PHH type) made by Tabai Corporation at temperature of tub set as 110degrees C., and it is kept to stand for 100 hours. Surface gloss valueof the surface with granulated leather embossed pattern of the pressmolded sheet before and after examination is measured using a digitalbending glossmeter (UGV-5DP type) made by Suga Test Instruments Co.,Ltd. under a condition in which incident angle-acceptance angle is setat 60 degrees, respectively. In addition, all gloss measurement isperformed after sample is cooled to room temperature.

In addition to (i) thermoplastic resins and (ii) olefin derivedcopolymers of the present invention both of which are indispensablecomponent, thermoplastic resin compositions of the present inventionsmay also contain one or more kinds of components selected from following(iii)-(v) in a range that does not impair an object of the presentinvention.

-   -   (iii): block copolymers consisting of polymer blocks mainly        containing vinyl aromatic compounds, and polymer blocks mainly        containing conjugated diene compounds,    -   (iv): hydrogenated (iii),    -   (v): ethylene derived polymers with a tensile strength at break        equal to or more than 2.1MPa measured based on JIS K6251.

(iii) maybe block copolymers consisting of polymer blocks mainlycontaining vinyl aromatic compounds, and polymer blocks mainlycontaining conjugated diene compounds. Polymer blocks mainly containingvinyl aromatic compound are polymer blocks that contain conjugated dienecompounds etc. as other constituent components. As vinyl aromaticcompounds, styrene, α-methyl styrene, p-methyl styrene, vinyl xylene,monochloro styrene, dichloro styrene, monobromo styrene, dibromostyrene, fluoro styrene, p-tert-butyl styrene, ethyl styrene, vinylnaphthalene, etc. may be mentioned. These are independently used, or twoor more of them are used in combination. Among these especiallypreferable compound is styrene. A content of vinyl aromatic compound inthe polymer block is preferably 60-99 weight %. When the content is toolittle, a mechanical strength of thermoplastic resin compositions and amolded body containing thermoplastic resin compositions may bedecreased. On the other hand, when the content is excessive, flexibilityof thermoplastic resin compositions and a molded body containingthermoplastic resin compositions may be decreased.

The polymer blocks mainly containing conjugated diene compounds arepolymer blocks that contain conjugated diene compounds as mainconstituent components, and vinyl aromatic compounds etc. as otherconstituent components. As conjugated diene compounds, 1,3-butadiene,isoprene, 2,3-dimethyl-1,3-butadiene, 2-neopentyl-1,3-butadiene, and2-chloro-1,3-butadiene, 2-cyano-1,3-butadiene, substituted linearconjugated penta dienes, linear chain and side chain conjugatedhexadienes, etc. may be mentioned. These are used independently, or twoor more of them are used in combination. Among these especiallypreferable compounds are 1,3-butadiene, and isoprene. A content ofconjugated diene compounds in the polymer blocks is preferably 60-99weight %. When the content is too little, flexibility of thermoplasticresin compositions and a molded body containing thermoplastic resincompositions may be decreased. On the other hand, when the content isexcessive, mechanical strength of thermoplastic resin compositions and amolded body containing thermoplastic resin compositions may bedecreased.

Specifically, (iii) is represented by a general formula: (cH-cS)n,(cH-cS)n-cH, and (cH-cS)n-X (where, in the formula, cH represents apolymer block mainly containing vinyl aromatic compounds, cS representspolymer block mainly containing conjugated diene compounds, and Xrepresents a coupling group residue, and n represents an integer of oneor more.)

A content ratio of ((polymer block mainly containing vinyl aromaticcompounds)/(polymer block mainly containing conjugated diene compounds))in block copolymers that consist of polymer blocks mainly containingvinyl aromatic compounds, and of polymer blocks mainly containingconjugated diene compounds is preferably 2/98-50/50. When the ratio istoo small, elasticity of thermoplastic resin compositions and a moldedbody containing thermoplastic resin compositions may be decreased, andhigh elasticity may not be obtained, and on the other hand, when theratio is too large, flexibility of thermoplastic resin compositions anda molded body containing thermoplastic resin compositions may bedecreased.

In order to obtain (iii), generally in organic solvent, block cH orblock cS is first polymerized using polymerization initiators, such asorganic lithium compounds, and subsequently, block cS or block cH may bepolymerized. Whichever of block cH or block cS may be polymerized first.Moreover, a block copolymer (cH-cS)n (n represents an integer of one ormore) may be obtained by repeating the polymerization operations. And,block copolymer cH-cS-cH may be obtained using polymerizationinitiators, such as organic lithium compound, by polymerizing block cH,and subsequently block cS, and further block cH in organic solvent. Whenthese operations is repeated, a block copolymer (cH-cS)n-cS (n is aninteger of one or more) may also be obtained. Thus, a block copolymer(cH-cS)n-X (X is coupling agent residue and n is an integer of one ormore) may also be obtained by adding a coupling agent to a thus obtainedblock copolymer (cH-cS)n. As coupling agents, diethyl adipate,divinylbenzene, tetrachloro silane, butyl trichlorosilane, tetrachlorotin, butyl trichloro tin, dimethyl dichloro silane, tetrachlorogermanium, 1,2-dibromo ethane, 1,4-chloro methyl benzene, bis(trichlorosilyl)ethane, epoxidized linseed oil, tolylene diisocyanate,1,2,4-benzene tri isocyanate, etc. may be mentioned. In addition,corresponding commercial materials may also be used as block copolymersmentioned in (iii) that contains polymer block mainly containing vinylaromatic compounds, and polymer block mainly containing conjugated dienecompounds.

(iv) is hydrogenated compounds of the above (iii). For example, theabove (iii) is dissolved into an inactive solvent, and hydrogenation isperformed to obtain (iv) under existence of a hydrogenation catalyst at20-150 degrees C. and under hydrogen pressure of 1-100 kg/cm²G. Rate ofhydrogenation of conjugated diene compound in the above-mentioned (iii)may be adjusted by changing conditions at the time of hydrogenationreaction, such as a hydrogenation catalyst, an amount added of ahydrogenation compound, or a hydrogen pressure and a reaction time. Inaddition, corresponding commercial materials may also be used ashydrogenated compounds of the above (iii) of (iv).

When a property excellent in flexibility and mechanical strength isrequired of thermoplastic resin compositions and a molded bodycontaining thermoplastic resin compositions of the present invention,the thermoplastic resin compositions and a molded body containing thethermoplastic resin compositions preferably satisfy conditions below.

-   -   (i) is contained of 1-98 weight %, (ii) is contained of 1-98        weight %, and    -   (iii) and/or (iv) are contained 1-98 weight %, and more        preferably (i) is contained of 5-90 weight %, (ii) is contained        of 5-90 weight %, and (iii) and/or (iv) are contained 5-90        weight %.

(v) is ethylene derived polymers whose tensile strength at breakmeasured based on JIS K6251 is 2.1 or more MPa. As examples of (v),low-density polyethylene, linear low-density polyethylene,super-low-density polyethylene, medium-density polyethylene,high-density polyethylene, and copolymer containing ethylene, that is,copolymers or multiple copolymers of ethylene with one or two comonomersor more selected form the following group may be mentioned. The group isshown below: alpha-olefins, such as ethylene, propylene, 1-butene,4-methyl-1-pentene, 1-hexene, 1-heptene, and 1-octene; non-conjugateddienes, such as 1,4-hexadiene, dicyclopentadiene, and5-ethylidene-2-norbornene; monocarboxylic acids, such as acrylic acid,methacrylic acid, ethyl acrylic acid, and crotonic acid; dicarboxylicacid and mono esters thereof, such as maleic acid, fumaric acid,itaconic acid, and citraconic acid; acrylic acid or methacrylic acidester, such as methylmethacrylate, methyl acrylate, and ethyl acrylate;vinyl esters and their ionomers of saturated carboxylic acids, such asvinyl acetate and vinyl propionate. These polymers or copolymers may bemixtures of two or more. Furthermore, (v) is ethylene derived polymerswith ethylene content of equal to 80 mol % or more preferably.

When a property excellent in resistance to low temperature is requiredof thermoplastic resin compositions and a molded body containingthermoplastic resin compositions of the present invention, thethermoplastic resin compositions and a molded body containing thethermoplastic resin compositions preferably satisfy followingconditions; (i) is contained of 1-98 weight %, (ii) is contained of 1-98weight %, and (v) is contained of 1-98 weight %, and more preferably (i)is contained of 5-90 weight %, (ii) is contained of 5-90 weight %, and(v) is contained of 5-90 weight %.

When a property excellent in flexibility, mechanical strength, andresistance to low temperature is required of thermoplastic resincompositions and a molded body containing thermoplastic resincompositions of the present invention, the thermoplastic resincompositions and a molded body containing thermoplastic resincompositions preferably satisfy following conditions; (i) is containedof 1-97 weight %, (ii) is contained of 1-97 weight %, (iii) and/or (iv)is contained of 1-97 weight %, and (v) is contained of 1-97 weight %,and more preferably (i) is contained of 5-85 weight %, (ii) is containedof 5-85 weight %, (iii) and/or (iv) is contained of 5-85 weight %, and(v) is contained of 5-85 weight %.

Rubber components other than (ii) may be blended suitably if needed tothermoplastic resin compositions and a molded body containingthermoplastic resin compositions of the present invention in addition toindispensable components (i) and (ii), for example, natural rubbers,poly butadienes, liquefied poly butadienes, polyacrylonitrile rubbers,acrylonitrile-butadiene copolymer rubbers, partially hydrogenatedacrylonitrile-butadiene copolymer rubbers, isobutylene-isoprene rubbers,polychloroprene rubbers, fluororubbers, chloro sulfonated polyethylenes,silicone rubbers, polyurethane rubbers, isobutylene-isoprene copolymerrubbers, halogenated isobutylene-isoprene copolymer rubbers, etc.

If needed, thermoplastic resin compositions and a molded body containingthermoplastic resin compositions of the present invention may be givencross-linkings by conventionally well-known methods such as, sulfurcross-linking, peroxide cross-linking, metal ion cross-linking, silanecross-linking, resin cross-linking, etc. As cross-linking agents,cross-linking agents generally used in curing of rubbers may be used,and cross-linking agents of sulfur, phenol resin, metal oxide, metalhydroxide, metal chloride, p-quinone-dioxime, or bismaleimide derivedagents etc. may be mentioned. Although cross-linking agents may be usedindependently, In order to adjust cross-linking velocity, cross-linkingaccelerators may be used together. Oxidizers, such as minium anddibenzothiazoylsulfide, may be used as cross-linking accelerators. Andas dispersants, metal oxide like zinc oxide, stearic acid, etc. may beused together. As metal oxides, zinc oxide, magnesium oxide, lead oxide,and calcium oxide may be used, and preferably zinc oxide or magnesiumoxide may be used. And, dynamic cross-link may be given to thermoplasticresin compositions of the present invention to obtain cross-linkedcompounds under existence of cross-linking agents.

Various stabilizers, such as age resistors, antioxidant, ozonedegradation inhibitors, UV absorbents, and optical stabilizers, may besuitably blended with thermoplastic resin compositions and a molded bodycontaining thermoplastic resin compositions of the present invention asadditional components. And, additives, such as antistatic agents, slipagents, internal release agents, colorants, dispersants, anti blockingagents, lubricants, and anticlouding agents, may be blended suitably.

Fillers, such as glass fibers, carbon fibers, metal fibers, glass beads,asbestos, mica, calcium carbonate, titanic acid potassium whiskers,talc, aramid fibers, barium sulfate, glass flakes, and fluororesins,mineral oil derived softeners, such as naphthene oil and paraffinderived mineral oils, etc. may be suitably blended with thermoplasticresin compositions and a molded body containing thermoplastic resincompositions of the present invention as addition components.

Flame retarder may be suitably blended with thermoplastic resincompositions and a molded body containing thermoplastic resincompositions of the present invention as addition components. Asexamples of flame retarders, inorganic compounds, such as antimonyderived flame retarders, aluminum hydroxide, magnesium hydroxide, zincborate, guanidine derived flame retarders, and zirconium derived flameretarders; phosphates and phosphorus compounds, such as poly phosphoricacid ammonium, ethylene bis-tris(2-cyano ethyl)phosphonium chloride,tris(tribromo phenyl)phosphate, tris(tribromo phenyl) phosphate, andtris(3-hydroxypropyl)phosphine oxide; chlorine derived flame retarders,such as chlorinated paraffin, chlorinated polyolefin, and perchlorocyclopentadecane, bromine derived flame retarders, such ashexabromobenzene, ethylene bisdibromo norbornane dicarboxyimide,ethylene bistetrabromo phthalimide, tetrabromo bisphenol A derivatives,tetrabromo bisphenol S, and tetrabromo dipentaerythritol, and thosemixtures may be mentioned.

Foaming agent may be blended with thermoplastic resin compositions and amolded body containing thermoplastic resin compositions of the presentinvention as an addition component to provide sponge-like products. Asexamples of foaming agents, body foaming agents, such as sodiumbicarbonate, ammonium bicarbonate, and ammonium carbonate; nitrosocompounds, such as N,N′-dinitroso pentamethylenetetramine; azocompounds, such as azocarbonamide and azpisobutylonitrile;sulfonylhydrazides, such as benzene sulfonylhydrazine, p,p′-oxybis(benzene sulfonylhydrazide), toluene sulfonylhydrazide, and toluenesulfonylhydrazide derivatives etc. may be mentioned. And in foamingprocessing, foaming auxiliary agents may be used suitably. As examplesof foaming auxiliary agents, salicylic acid, urea, and their compounds,etc. may be mentioned.

Polar polymers may be added as auxiliary agents for high-frequencyfabricating to thermoplastic resin compositions and a molded bodycontaining thermoplastic resin compositions of the present invention. Asexamples of polar polymers, copolymers or multiple copolymers ofethylene and one or more comonomers selected from the following group ofcompounds may be mentioned, that is; monocarboxylic acid, such asacrylic acid, methacrylic acid, ethyl acrylic acid, and crotonic acid;dicarboxylic acids, such as maleic acid, fumaric acid, itaconic acid,and citraconic acid; their monoester; acrylic acids, such asmethylmethacrylate, methylacrylate, and ethylacrylate; or vinyl estersof saturated carboxylic acid, such as methacrylic acid esters, vinylacetate, and vinyl propionate, and their ionomers.

In addition to (i) and (ii) that are indispensable component, otherresin components, for example, rosin derived resins, polystyrene derivedresins, synthetic petroleum resins, coumar one derived resins, phenolderived resins, xylene derived resins, styrene derived resins, isoprenederived resins, etc., may be blended suitably to thermoplastic resincompositions and a molded body containing thermoplastic resincompositions of the present invention, if needed. As rosin derivedresins, natural rosins, polymerized rosin, partially and fullyhydrogenated rosins; glycerine esters of these various rosins;esterified compounds, such as pentaerythritol esters, ethylene glycolesters, and methyl esters; and further, rosin derivatives modified bydisproportionation, fumarization, limization, or by suitably combinedmethods of these modification may be mentioned. As poly terpene derivedresin, homopolymers or copolymers of cyclic terpene, such as α-pinene,β-pinene, and dipentene; terpene-phenol derived resins, such asα-pinene-phenol resins, dipentene phenol resins, terpene-bisphenolresins, etc. that are copolymers of various kinds of above-mentionedterpene and phenol derived compounds, such as phenol and bisphenol;furthermore, aromatic modified terpene resins that are copolymers of thevarious above-mentioned terpenes and aromatic monomers may be mentioned.As synthetic petroleum resins, C₅ fractions and C₆ to C₁₁ fractions ofnaphtha cracking oil; homopolymers or copolymers of olefin derivedfractions; aliphatic derived petroleum resins, aromatic derivedpetroleum resins, cycloaliphatic derived petroleum resins,aliphatic-cycloaliphatic copolymerized resins that are hydrogenatedcompounds of these polymers, etc. may be mentioned.

Furthermore, copolymers of various kinds of above-mentioned naphthacracked oils and various above-mentioned terpene, copolymerizedpetroleum resins that are hydrogenated compounds may be mentioned. As C₅fractions of naphtha cracking oils here, methyl butene, such asisoprene, cyclopentadiene, 1,3-pentadiene, 2-methyl-1-butene, and2-methyl-2-butene; pentenes, such as 1-pentene and 2-pentene;dicyclopentadiene etc. are preferable. As C₆ to C₁₁ fractions, methylstyrenes, such as indene, styrene, o-, m- and p-vinyltoluene, and α- andβ-methylstyrene; methylindene, ethyl indene, vinyl xylene, propenylbenzene, etc. are preferable. In addition, as an olefin derivedfractions, butene, hexene, heptene, octene, butadiene, octadiene, etc.are preferable.

As phenol derived resins, alkylphenol resin, alkyl phenol acetyleneresins by condensation by alkyl phenol and acetylene, and these modifiedcompounds may be mentioned. Here, as these phenol derived resins,novolak type resins in which phenol is methylolized with acid catalyst,and resol type resins in which phenol is methylolized with alkalicatalyst may be mentioned.

As xylene derived resins, xylene-formaldehyde resin that consists ofm-xylene and formaldehyde, and modified resin in which a third componentis added to the resin to be reacted may be mentioned.

As styrene derived resins, low molecular weight polymer of styrene,copolymerized resin of α-methyl styrene and vinyltoluene, copolymerizedresins of styrene, acrylonitrile, and indene, etc. may be mentioned.

As isoprene derived resins, resins obtained by copolymerizing C₁₀cycloaliphatic compounds of dimerized isoprene with C₁₀ linear compoundsmay be mentioned.

In various kinds of above-mentioned resins that give tackiness, rosinderived resins, poly terpene derived resins, synthetic petroleum resins,etc. are preferable. From a viewpoint of transparency of a molded bodyusing olefin derived copolymer compositions obtained, resins withaliphatic and/or cycloaliphatic structure in these resins are morepreferable. Here, as especially preferable resins giving tackiness thathave aliphatic and/or cycloaliphatic structure: in rosin derived resinspartially and fully hydrogenated rosin and those derivatives; in polyterpene derived resins, homopolymers or copolymers of cyclic terpenes;in synthetic petroleum resins, hydrogenated copolymer of aliphaticderived petroleum resin, cycloaliphatic derived petroleum resin,aliphatic-cycloaliphatic copolymerized resins, naphtha cracked oils, andvarious terpene may be mentioned. These resin components are usedindependently, or in combination of mixture of two or more kinds. Inaddition, corresponding commercial materials may be used as resincomponents.

Thermoplastic resin compositions of the present invention may be used asmultilayered materials of two or more layers that have at least onelayer consisting of thermoplastic resin compositions of the presentinvention. Materials of layers in the laminated layers constituting eachlayer may be the same mutually or may be different from each other. Asmaterials constituting each layer, it is possible to be selected fromwell-known components of thermoplastic resins, rubbers, and othersbesides thermoplastic resin compositions of the present invention. Asthermoplastic resins among these materials, resins selected from afollowing group may be used: various ethylene derived resins, variouspolypropylene derived resins various polybutene derived resins, variouspolymethylpentene derived resins, polystyrene derived resins; copolymerresins of ethylene and acrylic acid derived monomers; copolymer resinsof ethylene and vinyl acetate derived monomers; copolymer resins ofethylene and methacrylic acid derived monomers; acrylate resins,polyester derived resins, polycarbonate derived resins, nylon derivedresins, polyvinylalcohol derived resins. As rubbers, various rubbercomponents other than copolymers of the present Invention may bementioned, for example, ethylene/α-olefin derived copolymer rubbers,ethylene/α-olefin/polyene derived copolymer rubbers, styrene derivedrubbers, hydrogenated styrene derived rubbers, diene derived rubbers,and well-known cross linked rubbers may be mentioned. As othercomponents, materials chosen from textiles, nonwoven fabric, etc.,various stabilizers, various additives, fillers, mineral oil derivedsofteners, flame retarders, high-frequency fabricating assistants, rosinderived resins, polyterpene derived resins, synthetic petroleum resins,coumarone derived resins, phenol derived resins, xylene derived resins,isoprene derived resins, etc. may be mentioned, and these may be blendedsuitably. And, various kinds of materials containing thermoplastic resincompositions of the present invention may be resin materials that aregiven cross-link with sulfur cross-linking, peroxide cross-linking,metal ion cross-linking, silane cross-linking, resin cross-linking, etc.by well-known method, and resin materials in which foaming agents areblended to receive sponge processing. In addition, adhesives to provideadhesive property may be inserted to between layers of multilayeredmaterials if needed.

As methods of obtaining thermoplastic resin compositions of the presentinvention, each component explained above may be kneaded using forexample, usual kneading equipment, rubber mills, Brabender mixers,Banbury mixers, pressurized kneaders, ruders, biaxial extruders, etc. Askneading equipment, both sealed system and open system may be used, butequipments by sealed system type that may be substituted by inert gasare preferable. Kneading temperature is a temperature at which all themixed constitution components are melted, and is usually 160-250 degreesC., and is preferably 180-240 degrees C. Although it is not generallydiscussed because of dependency on kinds of mixed constitutingcomponents, quantity, and kind of kneading equipments, kneading time isusually about 3-10 minutes, when using kneading equipments, such aspressurized kneader and Banbury mixers. In addition, in kneadingprocess, each constitutiing components may be collectively kneaded, anda multi-stage division kneading method in which after some constitutingcomponents are kneaded at a first, remaining constituting components areadded and kneading is continued is also employable.

It is preferable that thermoplastic resin compositions of the presentinvention have pellet-like shape in consideration of transfer ortransportation. Although known technology may be mentioned as methods ofpelletizing of thermoplastic resin compositions, and for example, afteruniformly molten, (i) thermoplastic resins and (ii) olefin derivedcopolymers are extruded by extruder, pellets in a shape of a globular,acylinder, and a lens are obtained by hot cutting or strand cutting. Inthis case, cutting may be carried out under any condition of aircurrents, underwater, in air, etc. Strands with dual structure, in which(i) thermoplastic resins as outer layer and (ii) olefin derivedcopolymers as inner layer are configured, may be obtained, and thuspellets that contain resins with low mutual adhesiveness may be suppliedeffectively, using equipments with system that can configure two-layeredstrands (inner layer and outer layer), with different polymers. And,after (i) thermoplastic resins and the (ii) olefin derived copolymersare molten and mixed uniformly, the mixture molded to obtain sheets withrolls etc. may be pelltized into cubic shape by sheet pelletizingmachine. Pellets preferably have a length of longest portion of 3 cm orless in size. In the case of pellets with size exceeding this size,measurement error may become larger.

Pellets comprising thermoplastic resin compositions of the presentinvention may be preferably powdered on their surface with one kind ormore of materials, such as calcium carbonate, barium sulfate, silica,talc, stearic acid, and poly olefin powder in the light of inhibition ofpellet-bridging phenomenon caused by coagulation. A mount of powderingmay be decided based on a size and a form of pellets, and it ispreferably 0.05-3 weight parts based on an amount of pellets ofthermoplastic resin compositions. Effect of stopping coagulation may bepoor if added amount is too small, and if too much, decrease in physicalproperties and manufacturing cost rise may be caused.

Thermoplastic resin compositions of the present invention are primarilyprocessed into various molding objects, such as pipe and joint, film,sheet, hose, inner tube, etc. using well-known methods, such asextrusion molding, variant extrusion molding, multi-color extrusionmolding, covering (with core) extrusion molding, injection molding,compression molding, foamed molding, hollow molding, powder molding,calender molding, kneading processing, and inflation. For example, as anexample of powder molding method, the slash molding method, the flowdipping method, electrostatic coating method, powder thermal sprayingmethod, the powder rotational molding method, etc. are mentioned. And,as for molded bodies that consist of thermoplastic resin compositions ofthe present invention, well-known surface treatment, such as paint andvacuum evaporation, can be performed. Moreover, the above-mentionedprimary products may further be processed to obtain commercial productsby processing, such as bending, cutting, cut forming, die cutting, diedrawing, sculpture, press processing, hot stamping, high-frequencyfabricating, ultrasonic processing, lamination, sewing/rolledseaming/hand-knit, vacuum forming, pneumatic molding, adhesion, welding,hair transplantation, lining processing, slit processing, and printing.

Although base material films or sheets of the present invention may betransparent and colorless, coloring or printing may be given to be used.

Although especially manufacturing process of base material sheets orfilms of the present invention is not limited, for example, after eachcomponent is kneaded with dry blend or usual kneading equipment, forexample, rubber mill, Brabender mixer, Banbury mixer, pressurizedkneader, ruder, biaxial extruder, etc. the material may be processed toobtain laminated films and sheets by inflation method, extruding methodby T type dice, uniaxial drawing method, biaxial drawing method,calender roll, etc. Although thickness of films obtained is notespecially limited, it is preferably 0.02-2 mm, and more preferablyabout 0.03-0.2 mm.

Moreover, pressure sensitive adhesive layer may be prepared on at leastone face of base material films of the present invention, or sheets toobtain tacky adhesion sheets or films may be provided. This pressuresensitive adhesive is not especially limited, and for example, rubberderived pressure sensitive adhesives, such as natural rubbers,ethylene-α-olefin copolymers, atactic polypropylenes, andpropylene-α-olefin copolymers, ethylene-vinyl acetate copolymers,polyamides, polyesters, polycarbonates, poly vinyl ethers, polyvinylalcohol, polyurethanes, styrene derived block copolymers,polyisobutylene-butyl rubber derivatives, and poly isoprene derivatives;acrylic derived pressure sensitive adhesives, such as graft polymerobtained by polymerization of the acrylics derived monomers, andcopolymers with 2-ethyl hexyl acrylate and butyl acrylate as mainmonomer; silicone derived pressure sensitive adhesives etc. may be usedas pressure sensitive adhesives in a form of solvent type, non-solventtype, emulsion type, water-soluble type, etc. Thickness of pressuresensitive adhesives usually has about 0.001-0.2 mm preferably. Moreover,softener, optical stabilizers (UV absorbent, quencher, etc.),antioxidant, anticorrosive, colorant, filler, age resistor,cross-linking agent, etc. may be added. Pressure sensitive adhesive maybe coated on base materials by coating machine, and pressure sensitiveadhesive layers are formed. In the light of environmental problems,working environment, etc. in these days, pressure sensitive adhesivelayers are preferably prepared using a hot-melt coating method on filmsand sheets of base material. Moreover, in this case, base materials andpressure sensitive adhesive layers may be processed by technologies,such as co-extrusion method and the extrusion coating method (it is alsocalled the extrusion laminating method), using inflation filmmanufacturing equipment, T die film manufacturing equipment, etc.

Furthermore, when using tacky adhesion sheets or films especially inrolls, it is preferable to reduce an affinity of tacky adhesion sheetsor films to opposite side of themselves in the light of what is calledreleasing-out property, i.e., self-releasing property. For this reason,release coated papers may be inserted or releasing agents may be coatedto a face opposite to a side in which pressure sensitive adhesive layeris given on base materials of tacky adhesion sheets or films.

EXAMPLE

Although the following examples describe the present invention stillmore concretely, these examples are for illustration and do not limitthe present invention. [1] Synthesis of Olefin Derived Copolymer

Example 1

Copolymerization of ethylene, propylene, 1-butene, and5-ethylidene-2-norbornene (ENB) was continuously performed usingpolymerization apparatus made of SUS of 100 L equipped with agitatingblades. That is, hexane was continuously supplied as a polymerizationsolvent from a lower part of polymerization apparatus at the rate of 83L/hour, and following raw materials were simultaneously supplied at eachvelocity continuously respectively; ethylene: 2.0 kg/hour; propylene:8.3 kg/hour: 1-butene: 12.7 kg/hour; and 5-ethylidene-2-norbornene(ENB): 6.3 kg/hour. On the other hand, from upper part of thepolymerization apparatus, polymerization liquid was continuouslyextracted so that the polymerization liquid in the polymerizationapparatus might be kept a level of 100 L. As catalysts, dimethylsilyl(tetramethylcyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium dichloride,triphenylmethyl tetrakis(pentafluoro phenyl)borate, triisobutyl aluminum(henceforth referred to as TIBA) were continuously supplied into thepolymerization apparatus at rates of 0.092 g/hour, 2.755 g/hour, and5.251 g/hour respectively from the lower part of the polymerizationapparatus. Moreover, molecular weight regulation was performed byhydrogen. Copolymerization reaction was performed at 50 degrees C. whilecirculating cooling water in a Jacket attached in exterior of thepolymerization apparatus. A small amount of ethanol was added into apolymerization liquid extracted from the polymerization apparatus, andpolymerization reaction was stopped. After monomer was stripped off andwashed with water, solvent was removed off by steaming in a large amountof water, and thus copolymer was taken out. Copolymer was dried at 80degrees C. day and night under reduced pressure. Thusethylene/propylene/1-butene/5-ethylidene-2-norbornene copolymerizationwas performed at a rate of 2.39 kg/hour by the above operation.

Comparative Examples 1 and 2

In Example 1, except that the amount of monomer added and amount ofcatalyst added as shown in Table 1 were used, the same method wasfollowed fundamentally and copolymer was obtained. Detailed result issummarized in Table 1.

Dimethyl silyl(tetramethylcyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium dichloride

[2] Analysis of Olefin Derived Copolymer

(1) IR Measurement

Copolymer obtained by Example 1 and Comparative examples 1 and 2 wereanalyzed by IR measurement. Methylene rocking vibration of ethylene at720 cm⁻¹, methyl group rocking vibration originated from methyl branchin propylene at 1154 cm⁻¹, and methyl group rocking vibration originatedfrom ethyl branch in 1-butene at 770 cm⁻¹ were observed. This shows thatcopolymerization of each monomer component was carried out.

(2) Intrinsic Viscosity [η]

Measurement of intrinsic viscosity was performed in 135-degree C.tetralin using Ubbelohde viscometer. Sample 300 mg was dissolved intetralin 100 ml, and 3 mg/ml of solution was prepared. Furthermore, thesolution concerned was diluted into concentration of 1/2, 1/3, and 1/5,and each diluted solution was measured in oil thermostat bath at 135degrees C. (±0.1 degrees C.). For each concentration, measurement wasrepeated 3 times and acquired value was averaged.

(3) Molecular Weight-distribution Measurement

Molecular weight distribution was measured by gel permeationchromatography (GPC) method (product made by Waters, 150 C/GPCequipment). Following condition was used; elution temperature: 140degrees C., Used column: Sodex Packed Column A-80M by Showa Denko K.K.,molecular weight standard substance: polystyrene (made by TOSOH CORP.molecular weight 68-8400000). Weight average molecular weight convertedinto polystyrene is defined as (Mw) and number average molecular weightas (Mn), and this ratio (Mw/Mn) is defined as molecular weightdistribution. About 5 mg of measurement sample polymer was dissolved ino-dichlorobenzene 5 ml to obtain a solution with a concentration ofabout 1 mg/ml. Obtained sample solution 400 μl was injected. Elutionsolvent flow velocities were 1.0 ml/min, and detection was carried outby a refractive index detecting element.

(4) Differential Scanning Calorimeter (DSC) Measurement

Measurement was performed at the rate of 10 degrees C./min in both oftemperature rising and constant process using a differential scanningcalorimeter (DSC 220C by SEIKO Electronic Ind., Co.)

(5) Measurement of 5-ethylidene-2-norbornene (ENB) Content

Olefin derived copolymer was molded by heat pressing into a film shapeof thickness of 0.5 mm. Subsequently, using infrared spectrometer, peaktransmittancy (wave number 1650 cm⁻¹) originated from5-ethylidene-2-norbornene origin was obtained, and5-ethylidene-2-norbornene content in olefin derived copolymer wascalculated.

[3] Evaluation of Thermoplastic Resin Composition

After preliminary kneading was performed for 2 minutes on condition thattemperature of 200 degrees C., and screw rotational frequency 10 rpmusing plasticorder PLV 151 type by Brabender company using combinationsshown in Tables 2-5, kneading is performed for 10 minutes by 80 rpm.Press molding was carried out based on JIS K6758, and sheets of thecomposition were prepared.

Characteristics of thermoplastic resin compositions described in Examplewere measured by the following methods.

(1) Tensile Test JIS K6251

-   -   Specimen form dumbbell-like No. 3 type    -   Elongation velocity 200 mm/min    -   Number of specimen 3

Result of irregular low elongation cutting is omitted in tensileelongation at break EB (%). Result which shows tensile elongation atbreak of 80% or less of median of measurement result was omitted, andnumerical value to which arithmetic mean of the remaining measurementresults is carried out was adopted.

(2) Haze JIS K7105 Method.

-   -   Press sheet of thickness of 1 mm was measured.        (3) Heat Run Test:

Except that examination temperature is set at 110 degrees C., andexamination time as 100 hours, examination was carried out based on airheating aging test (6.3) of JIS K6301 “6. Aging test.” Test pieces werehung down and heated in testing machine tub, and the pieces hung downwere kept so that they did not touch each other of touch any portion ofwall in the testing machine tub.

(4) Hardness: ASTM D2240

(5) Surface Character Stability:

Generating state of stickiness or cloudiness in the surface of thesample of before and after (3) heat run test was Judged.

-   -   1: Stickiness and cloudiness observed: Judgment X    -   2: Cloudyness observed: Judgment Δ    -   3: Neither stickiness nor cloudiness observed: Judgment ∘        (6) Resistance to Whitening:

Molded body of 1 mm thickness was cut by 1 cm×5 cm, and grade ofwhitening after bent at an angle of 180 degrees was observed and judgedby viewing.

-   -   1: Whitening observed: Judgment X    -   2: No whitening observed: Judgment ∘

[4] Calculation

Relationship between an tensile elongation at break EB (%) and a weightpercentage (Pa) of olefin derived copolymer in resin composition wasprocessed by curvilinear regression in thermoplastic resin compositionsobtained in Examples 2-7 in which olefin derived copolymers of thepresent invention and polypropylene derived resins were blended, andpolypropylene resin shown in Example 8. The following quintic regressionwas obtained. Rate of contribution (R²) showed 0.9997.EB=82108×Pa⁵−128621×Pa⁴+78018×Pa³−23605×Pa²+3754.3×Pa+539.94  (expression5)

(Expression 5) was processed by linear regression in an area ofPa=0.20-0.60, and an area of Pa=0.30-0.50 using method of least squares,and, as a result, multiple correlation coefficients R[2/6] and R[3/5],gradient S[2/6], and gradient S[3/5] were obtained. In addition, inlinear regression, as Pa, in section of Pa=0.20-0.60, relationship of 41points that were obtained by substituting numerical values with 0.01units containing 0.20 and 0.60 for (eq5) was used, and in section ofPa=0.30-0.50, relationship of 21 points that were obtained bysubstituting numerical value of 0.01 units containing 0.30 and 0.50 for(expression 5) were used.

Multiple correlation coefficient R[2/6], and R[3/5] gave the followingvalues, and satisfied the relationship of (expression 1).R[2/6]=0.4804R[3/5]32 0.8993R[3/5]−R[2/6]=0.4189 R[3/5]−R[2/6]≧0.15  (expression 1)

Gradient S[2/6] and S[3/5] gave the following values, and satisfied therelationships of (expression 2) and (expression 3).S[2/6]=54.29S[2/6]≧−800   (expression 2)S[2/6]−70.32S[3/5]−S[2/6]=−124.61S[3/5]−S[2/6}≦−50  (expression 3)

The same calculation method was used and each parameter value wascalculated from relationships between tensile elongation at break EB (%)and weight percentage (Pa) of olefin derived copolymers in resincomposition (Table 6), in thermoplastic resin compositions ofComparative examples 3-8 and Comparative examples 9-14 in which olefinderived copolymers of Comparative example 1 and Comparative example 2and polypropylene derived resins were blended, and polypropylene resinshown in Example 8.

Results showed that in thermoplastic resin compositions obtained usingolefin derived copolymers of the present invention, low hardness wasrealized, and whitening by bending was not observed, and hightransparency was demonstrated, and the compositions were confirmed to bematerials showing no aggravation of quality in surface property afterheat run test.

TABLE 1 Compara- Compara- tive tive Example 1 example 1 example 2 Run-1Run-2 Run-3 Polymerization ° C. 50 55 50 temperature Ethylene Kg/h 2.02.0 5.0 Propylene Kg/h 8.3 8.3 8.3 1-butene Kg/h 12.7 12.7 12.7 *1 ENBKg/h 6.3 0 0 *2 (f) g/h 5.251 1.584 1.584 *3 (g) g/h 2.755 0.276 0.276*4 (h) g/h 0.092 0.018 0.018 ENB content Iodine 28 0 0 value Crystalmelting ° C. None None None point Amount of crystal mj/mg None None Nonemelting calorie Crystallization ° C. None None None temperature Amountof heat of mj/mg None None None crystallization Intrinsic viscosity dl/g1.0 1.0 1.0 [η] GPC Mw/Mn 2.2 2.2 2.2 Tensile strength at MPa 0.02 0.120.08 break (JIS K 6251) *1 ENB: 5-ethylidene-2-norbornene *2 (f):triisobutyl aluminum *3 (g): triphenylmethyltetrakis(pentafluorophenyl)borate *4 (h): dimethylsilyl(tetramethylcyclopentadienyl)(3-tert-butyl-5-methyl-2-phenoxy)titanium dichloride

TABLE 2 Example 2 3 4 5 Run-1 wt % 20 30 40 50 PP-1 wt % 80 70 60 50 Pa0.20 0.30 0.40 0.50 Tensile elongation % 790 810 800 800 at break (JIS K6251) Surface character stability Before heat run — — — ◯ test Afterheat run — — — ◯ test Haze (1 mm % — — — 30.7 thickness) Hardness (ShoreD) — — — 42.7 Resistance to — — — ◯ whitening

PP-1: Propylene ethylene random copolymer resin containing ethylene 4.9weight % that has a character in which MI shows 0.88 (g/10 min) under acondition of 230 degree C. and 2.16 kg load, and 20-degree C. xylenesoluble component shows 5.2%

TABLE 3 Example 6 7 8 Run-1 wt % 60 70 0 PP-1 wt % 40 30 100 Pa 0.600.70 0.00 Tensile elongation % 860 1280 540 at break (JIS K 6251)Surface character stability Before heat run — ◯ ◯ test After heat run —◯ ◯ test Haze (1 mm % — 35.7 56.9 thickness) Hardness (Shore D) — 20.763.1 Resistance to — ◯ X whitening

PP-1: Propylene ethylene random copolymer resin containing ethylene 4.9weight % that has a character in which MI shows 0.88 (g/10 min) under acondition of 230 degree C. and 2.16 kg load, and 20-degree C. xylenesoluble component shows 5.2%

TABLE 4 Comparative example 3 4 5 6 7 8 Run-2 wt % 20 30 40 50 60 70PP-1 wt % 80 70 60 50 40 30 Pa 0.20 0.30 0.40 0.50 0.60 0.70 Tensileelongation % 880 840 890 880 930 1610 at break (JIS K 6251) Surfacecharacter stability Before heat run — — — — — ◯ test After heat run — —— — — X test Haze (1 mm % — — — — — 20.9 thickness) Hardness (Shore D) —— — — — 22.0 Resistance to — — — — — ◯ whitening

PP-1: Propylene ethylene random copolymer resin containing ethylene 4.9weight % that has a character in which MI shows 0.88 (g/10 min) under acondition of 230 degree C. and 2.16 kg load, and 20-degree C. xylenesoluble component shows 5.2%

TABLE 5 Comparative example 9 10 11 12 13 14 Run-3 wt % 20 30 40 50 6070 PP-1 wt % 80 70 60 50 40 30 Pa 0.20 0.30 0.40 0.50 0.60 0.70 Tensileelongation % 780 760 640 560 430 370 at break (JIS K 6251) Surfacecharacter stability Before heat run — — — — — ◯ test After heat run — —— — — ◯ test Haze (1 mm % — — — — — 90.3 thickness) Hardness (Shore D) —— — — — 16.3 Resistance to — — — — — X whitening

PP-1: Propylene ethylene random copolymer resin containing ethylene 4.9weight % that has a character in which MI shows 0.88 (g/10 min) under acondition of 230 degree C. and 2.16 kg load, and 20-degree C. xylenesoluble component shows 5.2%

TABLE 6 Run-1 + PP Run-2 + PP Run-3 + PP R[2/6] 0.4804 0.7897 0.9893R[3/5] 0.8993 0.9140 0.9979 R[3/5] − R[2-6] 0.4189 0.1243 0.0086 (◯) (X)(X) S[2/6] 54.29 133.83 −939.91 (◯) (◯) (X)

As is described above according to the present invention, thermoplasticresin compositions with outstanding flexibility, transparency,resistance to whitening, scratch resistance, and tensile elongationcharacteristics, and excellent balance of flexibility, heat resistance,and weather resistance, and outstanding surface character stability areprovided.

Availability in Industry

Thermoplastic resin compositions of the present invention may be usedwith the outstanding feature in many usage, for example, vehicles parts,electrical and electric equipment parts, electric wires, buildingmaterials, agricultural and fishery and horticulture articles, chemicalindustrial use articles, engineering works materials, industry andindustrial materials, furniture, stationeries, miscellaneous businessgoods article clothes, container and packaging articles, toys, leisurearticles, medical application articles, etc. As vehicles parts, forexample, automobile interior outer layer materials, such as interiordesign panels, doors, pillars, and air bag covers; automobile exteriorparts, bicycle parts, etc. such as, over fenders, crowding panels, roofrails, and side malls may be mentioned. As electrical and electricequipment parts, for example, electrical and instrument parts,electronic parts, weak electric current parts, household electricappliances components, refrigerator articles, lighting apparatus,various covers for electricity, etc. may be mentioned. As electricwires, plastics cables, insulated conductors, electric wire protectionmaterials, etc. may be mentioned. As building materials, for example,wall and ceiling material uses, such as ribs, baseboard, panels, andtarpaulins; roofing material uses, such as corrugated plates, waterpipes, and roof ground materials; floors use, such as threshold materialand tile components; waterproofing uses, such as joints, joint sticks,and water proofing sheets; equipment part uses, such as ducts, cableducts, prefab components, and septic tanks; structure and fixturesmaterial uses, such as edges for construction, gaskets for construction,carpet stoppers, angles, and louvers; industrial materials uses, such asjoiners and cure sheets may be mentioned. As agricultural, fishery, andhorticulture articles, house use for agriculture etc. is mentioned, forexample. As industrial materials, for example, machine covers, machineparts, packing, gaskets, flanges, leather canvas, bolts, nuts, valves,films for metal protection, etc. may be mentioned. As furniture,cabinets, stools, sofas, mats, curtains, tablecloths, etc. may bementioned, for example. As stationeries, card cases, writing implementcases, accessories, key cases, money card cases, stickers, labels, bookjackets, note covers, binders, notebooks, covers, files, cards,commuter's tickets, underlay, holds, magazine trays, albums, templates,writing implement axis, etc. may be mentioned. As daily necessaries anda miscellaneous goods article, bath lids, drainboards, buckets, clothescovers, bedding cases, umbrellas, umbrella covers, reed screens,needlework tools, shelf boards, shelf receptacles, frames, aprons,trays, tapes, strings, belts, bags, etc. may be mentioned, for example.As clothes, raincoat, raincoats, rain gear sheets, child leatherjackets, shoes, shoes covers, foot wears, gloves, ski wears, hats, andsub materials for hats etc. may be mentioned. As container and apackaging articles, food containers, garments packaging articles,packing/packaging materials, cosmetics bottles, cosmetics containers,medicine bottles, food bottles, bottles for chemicals, detergentbottles, containers, caps, food packs, laminating films, shrink filmsfor industry, business-use lap films. etc. may be mentioned, forexample. As a medical application articles, transfusion bags,continuation carrying type peritoneal dialysis bags, blood bags, etc.may be mentioned, for example.

Thermoplastic resin compositions of the present invention may be usedfor base material sheets or films, and tacky adhesion sheets or filmsthat are constituted by the base material sheets or films asindispensable components, utilizing excellent balance of flexibility,heat resistance, and excellent characteristics in weather resistance,and surface character stability, flexibility, transparency, resistanceto whitening. In detail, they may be used in variable fields, such as,surface protection film for prevention of blemish and soil at the timeof storage or transportation of stainless steel and aluminum boards,makeup ply woods, sheet steels, resin boards, glasses, constructionmaterials, home electronics, precision instruments, cars, etc., andprevention of getting damaged at the time of secondary processing ofbending processing or press processing; and base material sheets orfilms that can be used for constituting tape for fixation or union etc.at the time of packaging and packing; and further tacky adhesion sheetsor films comprising the base material sheets or films and pressuresensitive adhesive layers or film, etc.

1. An olefin derived copolymer satisfying the following requirements (1)and (2): (1) strength at breakage of the olefin derived copolymermeasured according to JIS K6251 is not more than 2.0 MPa, and (2) aresin composition consisting of the olefin derived copolymer and apolypropylene derived resin, which resin contains a 20° C.xylene-soluble part in an amount of not more than 20% by weight,satisfies the following expressions, (expression 1) and (expression 2),R[3/5]−R[2/6]≧0.15  (expression 1)S[2/6]≧−800  (expression 2) wherein R[3/5] and R[2/6] are multiplecorrelation coefficients of a primary straight line obtained by a methodconsisting of the steps of: (i) plotting a content by weight (Pa) of theolefin derived copolymer contained in the resin composition as ahorizontal axis, and plotting an elongation at breakage, EB (%) measuredaccording to JIS K6251, of the resin composition as a vertical axis toobtain a curve, (ii) quintic multiple-regressing the above-obtainedcurve to obtain a multiple regression formula, which formula essentiallycontains data of at least seven Pa points, Pa=0.00, 0.20, 0.30, 0.40,0.50, 0.60 and 0.70, and further in case of containing more than sevenPa points, all the Pa values essentially have mutually constantintervals of not more than 0.10; and (iii) approximating a multipleregression curve in the sectional regions of Pa=0.30-0.50 andPa=0.20-0.60 of the above-obtained multiple regression formula accordingto a method of least square to obtain the above-mentioned primarystraight line and wherein S[2/6] is a gradient of a primary straightline (formula) obtained by approximating the above-mentioned multipleregression curve in the sectional region of Pa=0.20-0.60 according to amethod of least square.
 2. A thermoplastic resin composition comprising:(i) 1-99% by weight of a thermoplastic resin, and (ii) 99-1% by weightof the olefin derived copolymer according to claim
 1. 3. A thermoplasticresin composition comprising the following (A) and (B) as essentialcomponents: (A) the thermoplastic resin composition according to claim2, and (B) at least one resin selected from the group consisting of arosin derived resin, a poly terpene derived resin, a synthetic petroleumresin, a coumarone derived resin, a phenol derived resin, a xylenederived resin, a styrene derived resin and an isoprene derived resin. 4.A pellet comprising the thermoplastic resin composition according toclaim 2 or 3 as an essential component.
 5. A molded article comprisingthe thermoplastic resin composition according to claim 2 or 3 as anessential component, which article is molded according to any onemolding method selected from the group consisting of an extrusionmolding method, a profile extrusion molding method, a multi-colorextrusion molding method, a covering (with core) extrusion moldingmethod, an injection molding method, a compression molding method, anexpansion molding method, a blow molding method, a powder moldingmethod, a calender molding method, a kneading processing and aninflation molding method.
 6. A sheet or a film comprising thethermoplastic resin composition according to claim 2 or
 3. 7. Alaminated material, which comprises at least one layer containing thethermoplastic resin composition according to claim 2 or
 3. 8. A basematerial sheet or a base material film comprising the thermoplasticresin composition according to claim 2 or
 3. 9. An adhesive sheet or anadhesive film comprising the base material sheet or the base materialfilm according to claim 8, which sheet or film has a pressure sensitiveadhesive layer on at least one face thereof.
 10. An olefin derivedpolymer according to claim 1, wherein said expression 1 is:R[3/5]−R[2/6]≧0.20.
 11. An olefin derived polymer according to claim 1,wherein said expression 1 is:R[3/5]−R[2/6]≧0.25.
 12. An olefin derived polymer according to claim 1,wherein said expression 1 is:R[3/5]−R[2/6]≧0.30.
 13. An olefin derived polymer according to claim 1,wherein said expression 1 is:R[3/5]−R[2/6]≧0.35.
 14. An olefin derived polymer according to claim 1,wherein said expression 1 is:R[3/5]−R[2/6]≧0.40.
 15. An olefin derived polymer according to claim 1,wherein said expression 2 is:S[2/6]≧−200.
 16. An olefin derived polymer according to claim 1, whereinsaid expression 2 is:S[2/6]≧−100.
 17. An olefin derived polymer according to claim 1, whereinsaid expression 2 is:S[2/6]≧−50.
 18. An olefin derived polymer according to claim 1, whereinsaid olefin derived copolymer is selected from the group consisting of:(1) olefin derived copolymers of ethylene and α-olefin with 3-20 carbonsas indispensable monomers with which one or more monomer componentschosen from polyene compounds, cyclic olefins, and vinyl aromaticcompounds are arbitrarily copolymerized, (2) olefin derived copolymersof ethylene and α-olefin with 4-20 carbons as indispensable monomerswith which one or more kinds of monomer components chosen from polyenecompounds, cyclic olefins, and vinyl aromatic compounds are arbitrarilycopolymerized. (3) olefin derived copolymers in which ethylene,propylene, and α-olefins with 4-20 carbons are indispensable monomerswith which one or more kinds of monomer components chosen from polyenecompounds, cyclic olefins, and vinyl aromatic compounds are arbitrarilycopolymerized, (4) olefin derived copolymers of propylene and α-olefinswith 4-20 carbons as indispensable monomers with which one or moremonomer components chosen from polyene compounds, cyclic olefins, andvinyl aromatic compounds are arbitrarily copolymerized, (5) olefinderived copolymers that consist of monomer units based on ethylene andα-olefins with 4-20 carbons, (6) olefin derived copolymers that consistof monomer units based on ethylene α-olefins with 4-20 carbons andpolyene compounds, (7) olefin derived copolymers that consist of monomerunits based on ethylene, α-olefins with 4-20 carbons, and cyclic olefincompounds, (8) olefin derived copolymers that consist of monomer unitsbased on ethylene, α-olefins with 4-20 carbons, and vinyl aromaticcompounds, (9) olefin derived copolymers that consist of monomer unitsbased on ethylene, α-olefins with 4-20 carbons, polyene compounds, andvinyl aromatic compounds, (10) olefin derived copolymer that consist ofmonomer units based on ethylene, propylene, and α-olefins with 4-20carbons, (11) olefin derived copolymers that consist of monomer unitsbased on ethylene, propylene, α-olefins with 4-20 carbons, and polyenecompounds, (12) olefin derived copolymers that consist of monomer unitsbased on ethylene, propylene, α-olefins with 4-20 carbons, and cyclicolefin compounds, (13) olefin derived copolymers that consist of monomerunits based on ethylene, propylene, α-olefins with 4-20 carbons, andvinyl aromatic compounds, (14) olefin derived copolymers that consist ofmonomer units based on ethylene, propylene, α-olefins with 4-20 carbons,polyene compounds, and vinyl aromatic compounds, (15) olefin derivedcopolymers obtained by copolymerizing propylene and α-olefins with 4-20carbons, (16) olefin derived copolymers that consist of monomer unitsbased on propylene, α-olefins with 4-20 carbons, and polyene compounds,(17) olefin derived copolymers that consist of monomer Units based onpropylene, α-olefins with 4-20 carbons, and cyclic olefin compounds,(18) olefin derived copolymers that consist monomer units based onpropylene, α-olefins with 4-20 carbons, and vinyl aromatic compounds,and (19) olefin derived copolymers that consist of monomer units basedon propylene, α-olefins with 4-20 carbons, polyene compounds, and vinylaromatic compounds.